Compositions of matter: system II

ABSTRACT

The present invention relates to new compositions of matter, particularly metals and alloys, and methods of making such compositions. The new compositions of matter exhibit long-range ordering and unique electronic character.

BACKGROUND OF THE INVENTION

According to modern quantum theory, the chemical and physical propertiesof substances arise fundamentally from electrodynamic interactions.Modifying these interactions can alter electronic structures and therebyendow the elements of the periodic table and their compounds with newproperties.

U.S. Pat. No. 6,572,792, which is incorporated herein by reference, toChristopher J. Nagel describes a process for modifying the electronicstructure of a material and of the products that are produced by theprocess. For example, this patent describes metals, such as copper,cobalt, nickel, and alloys thereof, that possess novel properties, suchas novel XRF patterns and magnetic properties. However, it is desired tofurther amplify or modify the effects achieved by the process.

SUMMARY OF THE INVENTION

The present invention relates to improved methods of modifying theelectronic structure of a material. The process includes the iterativeand/or cyclic addition of energy to a material.

In one embodiment, the present invention includes a method of processinga metal or an alloy of metals, comprising the steps of:

(1.) Melting the material;

(2.) Adding a carbon source to the material; and

(3.) Varying the temperature of the material between two temperaturesover one or more cycles, wherein the material remains at a temperatureabove the melting point during the entire step.

The process can further comprise one or more of the steps, in one ormore iterations or cycles:

(4.) Adding a flow of a gas (such as nitrogen, hydrogen and/or a noblegas) through the material;

(5.) Varying the temperature of the material between two temperaturesover one or more cycles, wherein the material remains at a temperatureabove the melting point during the entire step;

(6.) Adding a carbon source to the material; and/or

(7.) Holding the material with optional gas addition.

The process in a preferred embodiment involves one or more iterations orcycles of adding energy to a material in a supersaturated state withcarbon. In this embodiment, the process comprises, or further comprises,one or more of the steps, in one or more iterations or cycles:

(8.) Lowering the temperature of a molten material, wherein the materialbecomes supersaturated with carbon;

(9.) Varying the temperature of the material between two temperaturesover one or more cycles, wherein supersaturation with carbon ismaintained and the material remains at a temperature above the meltingpoint during the entire step, optionally in the presence of gas additionduring the entire step or any portion of the step (e.g., during one ormore or all of the steps wherein temperature increases or decreases);(10.) Holding the material at a selected temperature, optionally in thepresence of gas addition;(11.) Cooling the material, such that the material continues to besupersaturated with carbon and the material remains at a temperatureabove the melting point, optionally in the presence of gas addition;and/or(12.) Cooling the material to room temperature, thereby obtaining asolidified manufactured material.

In one embodiment, steps 8 and 9 (or 9 and 11) are performed andrepeated 1, 2, 3, 4 or more times, preferably 4 or more times.

In preferred embodiments, the improvement in the processes of theinvention comprises at least one of the following:

(a) the gas or gaseous addition (e.g., nitrogen, hydrogen, and/or noblegas) is added to the material through a lance set at a level above theliquid level;

(b) at least one of the gases or gaseous additions comprises a gasmixture;

(c) at least one of the gases has been exposed to radiation;

(d) current, e.g., AC or DC current, is added to the material in afurther step or during one or more of the above steps;

(e) during the cooling step, a gas is added to the material; and/or

(f) during the cooling step, the material is quenched with water whereinthe water is not stirred;

(g) at least one form of radiation has been filtered;

(h) the material is exposed to radiation in a further step or during oneor more of the above steps; and/or

(i) varying the reactor power (e.g., above normal holding power) betweentwo power levels over ½, one or more cycles.

Advantages of the present invention include a method of processingmetals into new compositions of matter and producing and characterizingcompositions of matter with altered physical and/or electricalproperties.

DETAILED DESCRIPTION OF THE INVENTION

U.S. Pat. No. 6,572,792 to Christopher J. Nagel describes a process formodifying the electronic structure of a material and to the productsthat are produced by the process. For example, this patent, which isincorporated herein by reference in its entirety, describes metals, suchas copper, cobalt, nickel, and alloys thereof, that are induced by theprocess to acquire novel properties, such as novel XRF patterns andmagnetic properties. As described in that patent, electromagneticchemistry is the science that affects the transfer and circulation ofenergy in many forms when induced by changes in electromagnetic energy.In empty space, a constant speed for light, independent of the frame ofreference (i.e., “each ray of light moves in the coordinate system ‘atrest’ with the definite velocity V independent of whether this ray oflight is emitted by a body at rest or a body in [uniform] motion”) asadvanced in “The Theory of Electrodynamics of Moving Bodies” (Einstein,1905) implicitly embeds a discrete partition between its associatedcoordinate system at rest and the reference systems that are relative toit. A topological description of this partition, satisfying thepostulates advanced in the above referenced paper, requires that whenthe electrodynamic components of matter are manipulated, discretechanges in energy exchange occur between meromorphic constructions whilecontinuous changes in energy exchange occur along holomorphic mappings.Harmonics governing the redistribution of energy are the vehicles bywhich changes in (material) properties, such as the magnitude and/or theorientation, can occur. Alignment of the electrodynamic componentinduces effects that may result in significant changes in the underlyingmaterial species: (1) alignment of atoms with the resultingdirectionality of physical properties; (2) alignment of energy levelsand the capability to modify harmonic structure, may establish physicalproperties conducive for energy transfer; (3) alignment of theelectrodynamic component includes the opening of pathways for freeelectron flow, and; (4) alignment of electrodynamic field phaseorientation.

The present invention relates to new materials and compositions ofmatter, and includes manufactured, or tailored, metals or alloys ofmetals. A “manufactured” or “tailored” metal or alloy is a metal oralloy, which exhibits a change in electronic structure, such as thatseen in a fluid or adjustable XRF spectrum. The American HeritageCollege Dictionary, Third Edition defines “fluid” as changing or tendingto change.

Metals of the present invention are generally p, d, or f block metals.Metals include transition metals such as Group 3 metals (e.g., scandium,yttrium, lanthanum), Group 4 metals (e.g., titanium, zirconium,hafnium), Group 5 metals (vanadium, niobium, tantalum), Group 6 metals(e.g., chromium, molybdenum, tungsten), Group 7 metals (e.g., manganese,technetium, rhenium), Group 8 metals (e.g., iron, ruthenium, osmium),Group 9 metals (e.g., cobalt, rhodium, iridium), Group 10 metals(nickel, palladium, platinum), Group 11 metals (e.g., copper, silver,gold), and Group 12 metals (e.g., zinc, cadmium, mercury). Metals of thepresent invention also include alkali metals (e.g., lithium, sodium,potassium, rubidium, and cesium) and alkaline earth metals (e.g.,beryllium, magnesium, calcium, strontium, barium). Additional metalsinclude aluminum, gallium, indium, tin, lead, boron, germanium, arsenic,antimony, tellurium, bismuth, thallium, polonium, astatine, and silicon.

The present invention also includes alloys of metals. Alloys aretypically mixtures of metals. Alloys of the present invention can beformed, for example, by melting together two or more of the metalslisted above. Preferred alloys include those comprised of copper, gold,and silver; tin, zinc, and lead; tin, sodium, magnesium, and potassium;iron, vanadium, chromium, and manganese; nickel, tantalum, hafnium, andtungsten; copper and ruthenium; nickel and ruthenium; cobalt andruthenium; cobalt, vanadium and ruthenium; and nickel, vanadium andruthenium.

The material can be added, or charged, to the reactor in a variety offorms. For example, where the material is a metal, it can be convenientto add the material as powder, flakes, pellets or ingots. The materialcan be charged all at once or in stages, including continuously duringthe initial melt or energy addition step.

The backspace of the reactor can be advantageously purged by a gas, suchas a gas, as described below, or other gas. Nitrogen is a convenient gasfor this purpose. In one example, a nitrogen flow is maintainedthroughout an entire method, such that a nitrogen pressure of about0.4-0.6 psig or about 0.5 psig is maintained. Alternatively, othergases, such as argon may be used for such purposes.

Carbon sources of the present invention include materials that arepartially, primarily, or totally comprised of carbon. Suitable carbonsources include graphite rods, graphite powder, graphite flakes,fullerenes, amorphous carbon, diamonds, natural gas, methane, ethane,propane, butane, pentane, and combinations thereof. A preferred carbonsource has a high purity (<50 ppm, such as <10 ppm, preferably <5 ppmimpurities). The carbon source is selected, in part, based on the systemto which it is added. In one example, graphite rods and graphite flakesare added in a sequential manner. In another example, the carbon sourcecan be added as a gas, such as through the introduction of methane.

Carbon sources can be contacted with the material for variable periodsof time. The period of time the carbon source is in contact with thematerial is the time between adding the carbon source and removing theundissolved carbon source. The period of time can be from about 0.5hours to about 12 hours, about 1 hour to about 10 hours, about 2 hoursto about 8 hours, about 3 hours to about 6 hours, about 3.5 hours toabout 4.5 hours, or about 3.9 hours to about 4.1 hours. Alternatively,the period of time can be from about 5 minutes to about 300 minutes,about 10 minutes to about 200 minutes, about 20 minutes to about 120minutes, about 30 minutes to about 90 minutes, about 40 minutes to about80 minutes, about 50 minutes to about 70 minutes, or about 59 minutes toabout 61 minutes. As can be seen above, the process of the inventionrelies in part upon the cyclic, iterative and/or harmonic addition ofenergy to the material. In general, the carbon contact period willcoincide with a cycle, series of cycles or iteration of steps.

A cycle of the present invention includes a period of time where theenergy of a material is varied between a first and second selectedenergy endpoints with a return to the first energy endpoint. A halfcycle is the completion of a single sweep or variant between a first andsecond energy endpoint. A full cycle is the completion of two sweepsbetween the first and second energy endpoints. A cyclic step refers tothe repetition of two or more cycles without substantially changing theendpoints of each sweep. Iterations generally refer to the repeating oftwo or more steps, such as a cyclic step in combination with a coolingstep.

An energy level, such as an endpoint, can often be conveniently measuredby the material's (e.g., metal's) temperature and/or the degree to whicha material (e.g., metal) is saturated with a second component (e.g.carbon). Over a period of time, varying the temperature involves aperiod of raising (or increasing) the temperature of a material (e.g.,metal or alloy) and a period when the temperature of a material (e.g.,metal or alloy) decreases (either passively, such as by convection orheat transfer to the surrounding environment, or actively, such as by amechanical means or cooling, e.g., quenching). The time period of eachsweep can be selected to produce a harmonic energy pattern. The timeperiod is also, in part, dictated by the rate of heating and coolingwhich is practical by the equipment (e.g., induction furnace) used, thematerial selected and the mass of material being processed. In someexperiments, a cycle comprising a 7 minute period to increase the energylevel (sweep up) and a 7 minute period to decrease the energy level(sweep down) was used. However, other time periods (e.g., 2, 3, 4, 5, 6,8, 9, 10, 20 or more minutes) can be used. Further, combinations can beused (7 minutes up and 5 minutes down). Where energy is added to amaterial by other means (e.g., ultraviolet or infrared radiation,current or reactor power), the time periods are not limited by the rateof heating or cooling the material.

Increasing the temperature of the metal or alloy increases the amount ofcarbon that can be dissolved into that metal or alloy, which thereforedecreases the degree to which the metal or alloy is saturated withcarbon (relative to the temperature and degree of carbon saturation whengraphite saturation assemblies are removed the first time). Similarly,decreasing the temperature of the metal or alloy increases the(relative) degree to which the metal or alloy is saturated with carbon.Thus, carbon saturation levels of a material can also be used to measureor determine energy endpoints. Where the material to be modified is anon-metal (e.g., carbon, gas), the energy endpoints are better measuredby temperature or associated emission spectra.

A cycle can also include, or be interrupted or ended with, a holdingstep. Thus, the material can be held at an energy level (as measured,for example, by the temperature or degree of carbon saturation) for aselected period of time. The holding period can be several minutes toseveral hours or more. In one example, the material was held for 60minutes. In another example, the material was held for 5 minutes. Morethan one hold step can be incorporated into the process and can beincluded in an iteration of steps.

The degree to which a metal is saturated with carbon varies over thecourse of the process, as well as within a step. For example, the degreeof carbon saturation can vary between 70% and 95% in the first cyclingstep, between 80% and 95% in the second cycling step, between 101% and103% in the third cycling step, between 104% and 107% in the fourthcycling step, between 108% and 118% in the fifth cycling step, andbetween 114% and 118% in the sixth cycling step. It is preferred toconduct 4 or more supersaturation steps. Supersaturation is definedherein as follows:

-   -   ⁺n%_(wt), represents the weight percent above the equilibrium        saturation value of the material in its natural state. For        example, +1%_(wt) represents 1%_(wt) above the saturation value        as defined in its natural or naturally occurring state.    -   [n]_(eqsat) represents the equilibrium saturation of “n” in its        natural state. For example, [C]_(eqsat) represents the        equilibrium saturation of carbon for the thermodynamic state        specified (e.g., T, P, composition) when the composition is in        its natural, or naturally occurring, state.

Gas, such as nitrogen, hydrogen or a noble gas, can be added during acycle, except where it is specified that gas addition is ceased prior tothat cycle. The gas provides a third body effect for the reactionfacilitating energy exchange. For example, hydrogen, helium, nitrogen,neon, argon, krypton, xenon and carbon monoxide can be added. In apreferred embodiment, the gas is added as a mixture. A preferred mixturecomprises argon, helium, neon and/or krypton. Preferably, at least 50%,more preferably at least 80% such as at least 90% by volume argon,helium or hydrogen is present in the mixture. Particularly preferredmixtures, by volume, include (1) 93% argon, 5% helium and 2% neon; (2)92% argon, 5% helium and 3% neon; (3) 95% argon and 5% helium or neon;(4) 95% helium and 5% krypton; (5) 95% nitrogen and 5% helium; (6) 97%helium and 3% neon (optionally trace amounts of krypton); (7) 97% argonand 3% neon; (8) 60% argon and 40% helium (optionally trace amounts ofneon, hydrogen and/or krypton); (9) 49.5% hydrogen, 49.5% helium and 1%neon. In selecting the specific combination and concentrations of thegases, the following factors should be considered: emission profile,Hodge spectral character and required momentum/energy exchange.

In each embodiment, the gas can be added at various rates. In general,the gas is added in terms of the resulting agitation on the material andexchange with the material. As such, the gas can be added at a low rate,resulting in low agitation/exchange; at a modest, moderate or high orvigorous rate. The gases can be mixed prior to adding or addedindividually. Using conventional fluid dynamic scaling models andassuming a crucible size of 3.75 inches I.D., with a 14.5 inch height,holding 20 lbs of cobalt, examples of low agitation can be achieved byadding about 0.25 SLPM; modest agitation can be achieved by addingbetween about 1.25 SLPM; moderate agitation can be achieved by addingbetween about 2.5 SLPM and high agitation can be achieved agitation byadding between about 5.0 SLPM. Selecting low agitation generally resultsin clearly defined bubbles in a quiescent bath. High agitation generallyresults in a turbulent well-mixed bath. Modest and moderate agitationrates enables mixing and exchange to be adjusted between these extremes.In some instances, the rate of addition can begin at one level and bechanged during the step to a different level (e.g., from a low rate to avigorous rate). In general, it is desirable to add the gas at a rate ofexcess to assist in controlling the reaction and ensuring that ratelimiting steps are not associated with mass transfer diffusion. Flowrates for a crucible size of 8.875 inches, with a 16.5 inch height,holding 100 lbs of copper can be determined using standard scalingtechniques based on bubble size and residence time distributions toachieve similar transport phenomena.

The gas can be added to the material either below or above (includingacross) the surface level of the material. When the gas is added belowthe surface level, it can be added via injection ports from the bottomor sides of the reactor. However, it is often preferred to add the gasvia a lance. The lance can be positioned to provide gas entry below thesurface level, e.g. at the bottom of the reactor, midpoint or near thesurface of the material. When the lance is to be submerged, it is oftendesirable to position the lance prior to or during the initial chargingof the reactor with the material (e.g., as the reactor is being packedwith metal pellets). Where the lance is not submerged, the lance can beplaced to direct the gas across the surface of the material or toward atthe surface. Where the gas is directed toward the material, the gas canbe directed at a force that creates an indentation in the surface. Thelance can be placed along the centerline of the reactor. However, it isoften desirable to place the lance off center, e.g., at about two thirdsradius point as measured from the center. Lance placement involvesconsideration of mass/energy transfer, interaction of multiple lances,and harmonic character of the reactants being added.

The material can be subjected or exposed to the gas either during theentire process or a cycle or series of cycles or alternating cycles,during the cooling step or thereafter as a post treatment step.

Superior results in controlling the reaction have been achieved byexposing at least one gas to radiation. The exposure can be applied in acontinuous or batch mode. For example, the radiation source can beapplied as the gas moves through a conduit for the gas source to thereactor. The conduit is preferably not opaque and is more preferablytranslucent or transparent. The radiation can be applied in an open orclosed system. A closed system entails exposing the gas to the specifiedradiation in the substantial absence of other radiation sources (e.g.,visible light, magnetic fields above background). This can be easilyaccomplished by building a black box surrounding a segment of theconduit and placing the radiation source(s) within the black box. Anopen system can also be employed where the radiation source(s) are notshielded from ambient light.

In yet other embodiments, the material itself can be subjected toradiation, either during or after the processes described herein. Forexample, a tailored metal can be subjected to radiation to furthermodify the properties of the metal.

The radiation sources can be selected to provide a broad range ofemitted wavelengths. For example, the radiation can range from infraredto ultraviolet wavelengths. In one embodiment, examples of preferredradiation sources emit into the range of 160 nm to 1000 nm; in anotherembodiment, examples of preferred radiation sources emit and into therange of 180 nm to 1100 nm; and in a more preferred embodiment examplesof preferred radiation sources emit into the range of 400 nm to 700 nm.The radiation can be conveniently supplied by short arc lamps, highintensity discharge lamps, pencil lamps, lasers, light emitting diodes,incandescent, fluorescent, and/or halogens for example. Examples ofsuitable high intensity discharge lamps include mercury vapor, sodiumvapor and/or metal halide. Short arc lamps include mercury, xenon ormercury-xenon lamps. Pencil lamps include neon, argon, krypton, xenon,short wave ultraviolet, long wave ultraviolet, mercury, mercury/argon,mercury/neon, and the like. The radiation can also include (or exclude),incandescent or fluorescent light and/or natural sources of light, suchas electromagnetic radiation emitted by celestial bodies.

The radiation sources can optionally be used in combination with lightshields or wavelength filters. Examples of suitable shields and filterscan be obtained from UVP, Inc. (Upland, Calif.). The filters and shieldscan direct or modify the emission output. Examples of UVP Pen-RayFilters include the G-275 filter which absorbs visible light whiletransmitting ultraviolet at 254 nm and the G-278 filter which convertsshortwave radiation to longwave radiation at 365 nm. Pen-Ray Shieldsinclude Shield A which has a 0.04 inch ID hole for point-like source,Shield B which has a 0.31×0.63 inch window, and Shield C which has a0.19×1.5 inch window. Filters and shields can also be obtained fromNewport Corp. (Irvine, Calif.). The Newport 6041 Short Wave Filterabsorbs visible lines; the 6042 Long Wave Conversion Filter attenuatesthe 253.7 nm Hg line and fluoresces from 300-400 nm; and the 6057 GlassSafety Filter absorbs the 253.7 nm Hg line and attenuates the 312.6 nmline. The Aperture Shields offered by Newport include the 6038 PinholeShield which has a 0.040 inch (1 mm) diameter, the 6039 Small ApertureShield which has a 0.313×0.375 inch window and the 6040 Large ApertureShield with a 0.188×1.50 inch window. Filters and shields can also beobtained from Edmund Industrial Optics Inc. (Barrington, N.J.). TheEdmund UV Light Shield A has a 1 mm inner diameter drilled hole; ShieldB has a 7.9 mm×15.9 mm aperture; and Shield C has a 4.8 mm×38.2 mmaperture.

The orientation of the lamp can also impact upon the result obtained.Thus, in the embodiment where a gas is subjected to a radiation source,the radiation source can be fixed to direct the radiation directlytowards, perpendicular, away or parallel to the conduit directing thegas, or its entry or exit point. The gases can be those discussed aboveor other gases, such as air or oxygen. The radiation source can bepositioned horizontally, vertically and/or at an angle above, belowacross from the conduit. For example, the base of a pencil lamp (orother radiation source) can be set at the same height of the conduit andthe tip of the lamp directed or pointed toward the conduit.Alternatively, the base of the pencil lamp (or other radiation source)can be set at the height of the conduit and the lamp directed at a 30°(40°, 45°, 50°, 55°, 60°, or 90°) angle above (below) the conduit, thebase of the pencil lamp can be fixed above or below the level of theconduit. The tip of the pencil lamp can be pointed up or down, in thedirection of the gas flow or against the gas flow or at another anglewith respect to any of the above. Further, more than one of the same ordifferent pencil lamps alone or in combination with other radiationsources can be used, set at the same or different heights, orientationsand angles. The lamps can be presented in alternative orders (firstxenon, then mercury or vice versa).

In an embodiment wherein the material to be treated is subjected to theradiation source, similar positions can be achieved as above withrespect to the gas conduit. The radiation source can be fixed to directthe radiation directly towards, perpendicular, away or parallel to thematerial. The radiation source can be positioned horizontally,vertically and/or at an angle above, below across from the material. Asabove, the base of a pencil lamp (or other radiation source) can be setat the same height of the material and the tip of the lamp directed orpointed toward the material. Alternatively, the base of the pencil lamp(or other radiation source) can be set at the height of the material andthe lamp directed at a 30° (40°, 45°, 50°, 55°, 60°, or 90°) angle above(below) the material. Alternatively, the base of the pencil lamp can befixed above or below the level of the material. The tip of the pencillamp can be pointed up or down, in the direction of the gas flow oragainst the gas flow or at another angle with respect to any of theabove. Further, more than one of the same or different pencil lampsalone or in combination with other radiation sources can be used, set atthe same or different heights, orientations and angles.

In a preferred embodiment, the radiation source is a high intensitydischarge lamp positioned to direct the radiation towards the material.The high intensity discharge lamp is combined with one or more pencillamps positioned proximal to the high intensity discharge lamp. Often,high intensity discharge lamps are equipped with a hood or reflector todirect the radiation. In some instances, one or more pencil lamps can beplaced inside and/or behind the reflector.

Further, the distance between the radiation source and the materialand/or gas conduit can impact the results achieved. For example, thelamps can be placed between about 5 and 100 cm or more from the conduitand/or material. In other embodiments, the distance between theradiation source and the material and/or gas conduit can be betweenabout 100 cm and 5 meters or more.

In other instances, the radiation can be filtered. Filters, such ascolored glass filters, available from photography supply shops, forexample, can be used. In yet other embodiments, the filter can be othermaterials, such as water, gas (air or other gas), a manufactured ortailored material, such as those materials described or made herein, ora material of selected density, chemical make-up, properties orstructure. In one embodiment, the filter can be placed between theradiation source(s) and the target metal or alloy or gas used in themethod. Filters can also be called “(harmonic) forcing functions.”Forcing functions can be used in conjunction with electromagneticradiation sources to affect a change in a material. In addition, gasesmay be injected into apparatus containing a forcing function to modifythe performance of the assembly.

In one embodiment, the radiation source has an environment which isdifferent from that of the material. This can be accomplished bydirecting a gas flow into the lamp environment. Where the radiationsource is a pencil lamp within a box to radiate a gas, this can beaccomplished by direct gas flow into the box. In other embodiments, theradiation source can be a short arc lamp or a short arc lamp assembly.In such embodiments, the gas can be introduced into the reflectorproximate to the lamp. The gas includes those gases discussed above.

The radiation can be applied continuously or discontinuously (e.g.pulsed or toggled) and its intensity can be modulated. Where theradiation is applied continuously, the radiation can begin prior tointroduction of the gas into the conduit or after. It can be applied forthe duration of a cycle or series of cycles. Where the radiation ispulsed, the length of each pulse can be the same or different.Generally, the radiation is applied to induce harmonic change, alteringthe gas or target materials prior to their introduction into thereactor. This is conveniently accomplished by controlling the lamps witha computer. The factors to be considered in radiation source placement,exposure and sequence include the desired wavelength, intensity, andenergy characteristics, the angle of incidence, and the harmonic profileto be injected into the targeted material (e.g. gas, metal, tailoredmetal, radiated gas and the like).

In some instances, the radiation source and/or pencil lamp(s) and/orfilters and/or target material or gas are advantageously cooled. Forexample, where a high intensity discharge lamp is used in combinationwith a pencil lamp(s), it may be advantageous to cool the pencil lamp toprevent damage. Alternatively, where a short arc lamp is used incombination with pencil lamps and/or glass filters it may beadvantageous to cool the pencil lamps to prevent damage as well as theglass filter to prevent breakage.

Other sources of energy can be used to further tailor the materials ofthe invention. For example, DC current can be applied continuously orthe amperage varied, for example between 0-300 amps, such as 0-150 amps.AC current can be applied continuously or varied, e.g., in a wavepattern, such as a sinusoidal wave, square wave, or triangle wavepattern of a selected frequency and amplitude. Typically, 10 volts, peakto peak, is used at 0-3.5 MHz, 0-28 MHz, or 0-50 MHz. In otherembodiments, the peak to peak voltage was less that about 15 vdc, 10vdc, 8 vdc, 7.2 vdc, 5 vdc, 1.7 vdc, and 1 vdc. In one embodiment,electrodes can be placed in the reactor, such as below the surface ofthe material, and current applied. As with the radiation discussedabove, the current can be applied to coincide with a cycle or series ofcycles or during all or a part of a single step of the process. Oftenthe power supply is turned on prior to attachment to the electrodes toavoid any power surge impacts.

Further, the cooling step can alter the results of the process. Suchcooling can include gradual and/or rapid cooling steps. Gradual coolingtypically includes cooling due to heat exchange with air or other gasover 1 to 72 hours, 2 to 50 hours, 3 to 30 hours, or 8 to 72 hours.Rapid cooling, also known as quenching, typically includes an initialcooling with air or other gas to below the solidus temperature, therebyforming a solid mass, and placing the solid mass into a bath comprisinga suitable fluid such as tap water, distilled water, deionized water,other forms of water, gases (as defined above), liquid nitrogen or othersuitable liquified gases, a thermally-stable oil (e.g., silicone oil) ororganic coolant, and combinations thereof. The bath should contain asuitable quantity of liquid at a suitable temperature, such that thedesired amount of cooling occurs. The ingot can be removed from thecrucible before or after completing the cooling. While the material iscooling, the environment can be stirred, mixed or agitated. This can beaccomplished by maintaining a flow of coolant over the material, oragitating the cooling bath or environment. Alternatively, the coolant isnot disturbed or agitated and circulation of the coolant is minimized.

In one embodiment, the material is cooled in a different vessel (coolingor quench chamber). The cooling chamber can be, for example, apolyethylene (or other plastic) container. The ingot can be placeddirectly, or indirectly, into the cooling vessel (e.g., in a vertical orhorizontal orientation). Generally, the ingot can be placed at leastabout 6 inches from the inside wall of the container. The height of thecoolant can be at least about 12 inches above and below the surface ofthe ingot. A refractory material (e.g., a ceramic block rinsed withcoolant (e.g., DI water) and, optionally dried or allowed to dry) may beused to support the ingot in the quench chamber.

Where the material is cooled in a different vessel from the reactor orinduction furnace, the material can be removed, manually or robotically,to a clean, protected surface. This removal may be accomplished manuallyusing a pair of tongs (e.g. cast iron, steel, stainless steel, nickel,titanium, tungsten or other high temperature melting transition metal).Manual removal can also be accomplished by donning heavy, insulated,heat resistant gloves.

Where the crucible is removed from the reactor with the material, thecrucible should be removed before or after cooling. The crucible can beremoved by gently peeling it away from the material. A hammer, ram orwedge can be used to perform this function. However, care should be usedto avoid striking the material hard with the hammer or otherwise causinga substantial impact upon or metal contact with the material. In oneembodiment, the crucible removal can be performed in the presence of airat about 350±75° F., 750±250° F., 1100±250° F., or at T_(solidus) −75°F., T_(solidus) −5° F.

One example of the base method can be described in terms of carbonsaturation values. After a metal or alloy is added to a suitablereactor, establish the dissolved carbon level at 70% to 95% of theequilibrium saturation of carbon for the thermodynamic state specified(e.g., T, P, composition) when the composition is in its natural state(hereinafter the equilibrium saturation of carbon is referred to as“[C]_(eqsat)”). Identify temperature set points for 80% and 95%[C]_(eqsat). Vary the temperature between the predetermined set points,such that the temperature is decreased for 7 minutes and increased over7 minutes per cycle, for 15 cycles. Next, establish a flow of argon.Vary the temperature between the predetermined set points, such that thetemperature is decreased for 7 minutes and increased over 7 minutes percycle, for 5 cycles; the temperature should be maintained above 70%[C]_(eqsat) at all times and maintained below 95% [C]_(eqsat) at alltimes. The carbon level is raised to saturation (i.e., [C]_(eqsat)) withcontinued argon addition. Hold for 60 minutes at saturation (i.e.,[C]_(eqsat)) with continued argon addition. Raise the carbon level to⁺1%_(wt) (i.e., +1%_(wt) represents 1%_(wt) above the saturation valueas defined in its natural equilibrium state, [C]_(eqsat)) of [C]_(eqsat)with continued argon addition and hold for 5 minutes. Vary thetemperature for 20 cycles between ⁺1%_(wt) and ⁺3%_(wt) of [C]_(eqsat),such that the temperature is decreased over 9 minutes and increased over9 minutes per cycle. Cease argon addition. Cool the metal to ⁺4%_(wt) of[C]_(eqsat). Vary the temperature for 4.5 cycles between ⁺4%_(wt) and⁺70%_(wt) of [C]_(eqsat), such that the temperature is decreased over 3minutes and increased over 5 minutes. Argon is added as the carbonsaturation increases and nitrogen is added as carbon saturationdecreases. Cool the metal to obtain ⁺8%_(wt) with continued argonaddition. Vary the temperature over 15.5 cycles between ⁺80%_(wt) and⁺18%_(wt) of [C]_(eqsat), such that the temperature is decreased over 15minutes and increased over 15 minutes. Argon is added as the carbonsaturation increases and nitrogen is added as carbon saturationdecreases. After the 15.5 cycles are complete, gas addition is halted.Perform one complete cycle by varying the temperature between ⁺18%_(wt)to ⁺14%_(wt) of [C]_(eqsat) (ending at ⁺18%_(wt)), such that thetemperature is increased over 15 minutes and decreased over 15 minutes.Proceed immediately to a cool down that leads to solidification. Thepresent process also includes one or more of the further improvementsdescribed above.

Cycles of the present invention can vary in duration. The duration of acycle can vary among cycles in a step. A cycle duration is, for example,about 2 minutes to about 90 minutes, about 3 minutes to about 67minutes, about 5 minutes to about 45 minutes, about 8 minutes to about30 minutes, about 10 minutes to about 20 minutes, about 14 minutes toabout 18 minutes, about 7 minutes to about 9 minutes, about 13 minutesto about 15 minutes, about 17 minutes to about 19 minutes, about 28minutes to about 32 minutes, or about 29 minutes to about 31 minutes.

A cycle can be symmetric or asymmetric. In a symmetric cycle, the periodof increasing the metal or alloy temperature is equal to the period ofdecreasing the metal or alloy temperature. In an asymmetric cycle, theperiod of increasing the metal or alloy temperature is different thanthe period of decreasing the metal or alloy temperature. For anasymmetric cycle, the period of increasing the metal or alloytemperature can be longer than or shorter than the period of decreasingthe metal or alloy temperature.

For example, in a cycle lasting about 7 minutes to about 9 minutes, thetemperature can be increased for about 3 minutes and the temperature canbe decreased for about 5 minutes. If the cycle lasts about 13 minutes toabout 15 minutes, the temperature can be increased for about 7 minutesand the temperature can be decreased for about 7 minutes. If the cyclelasts about 17 minutes to about 19 minutes, the temperature can beincreased for about 9 minutes and the temperature can be decreased forabout 9 minutes. If the cycle lasts about 29 minutes to about 31minutes, the temperature can be increased for about 15 minutes and thetemperature can decreased for about 15 minutes.

The number of cycles in a step is generally an integer or half-integervalue. For example, the number of cycles in a step can be one or more,one to forty, or one to twenty. The number of cycles can be 1, 2, 3, 4,5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23,24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, or 40 ormore. Alternatively, the number of cycles in a step can be 0.5, 1.5,2.5, 3.5, 4.5, 5.5, 6.5, 7.5, 8.5, 9.5, 10.5, 11.5, 12.5, 13.5, 14.5,15.5, 16.5, 17.5, 18.5, 19.5, 20.5, 21.5, 22.5, 23.5, 24.5, 25.5, 26.5,27.5, 28.5, 29.5, or 30.5 or more. In a step comprising a half-integeror a non-integer quantity of cycles, either heating or cooling can occurfirst.

After the initial heating step, the temperature of a metal or an alloyis sufficiently high, such that the temperature is equal to or greaterthan the solidus temperature. The solidus temperature varies dependingon the metal or the alloy, and the amount of carbon dissolved therein.The temperature at the end of Step (F.) of the third paragraph of thesummary is typically about 900° F. to about 3000° F., but varies frommetal to metal. For example, the temperature at the end of Step (F.) canbe about 1932° F. to about 2032° F., about 1957° F. to about 2007° F.,or about 1932° F. to about 2467° F. for copper; about 2368° F. to about2468° F., about 2393° F. to about 2443° F., or about 2368° F. to about2855° F. for nickel; about 2358° F. to about 2458° F. or about 2373° F.to about 2423° F., or about 2358° F. to about 2805° F. for cobalt; about1932° F. to about 2032° F., about 1957° F. to about 2007° F., or about1932° F. to about 2467° F. for a copper/gold/silver alloy; about 399° F.to about 499° F., about 424° F. to about 474° F., or about 399° F. toabout 932° F. for a tin/lead/zinc alloy; about 399° F. to about 499° F.,about 424° F. to about 474° F., or about 399° F. to 932° F. for atin/sodium/potassium/magnesium alloy; about 2550° F. to about 2650° F.,about 2575° F. to about 2625° F., or about 2550° F. to about 2905° F.for silicon; about 2058° F. to about 2158° F., about 2073° F. to about2123° F., or about 2058° F. to about 2855° F. for iron; about 2058° F.to about 2158° F., about 2073° F. to about 2123° F., or about 2058° F.to about 2855° F. for an iron/vanadium/chromium/manganese alloy; or2368° F. to about 2468° F., about 2393° F. to about 2443° F., or about2368° F. to about 2855° F. for a nickel/tantalum/hafnium/tungsten alloy.

Methods of the present invention are carried out in a suitable reactor.Suitable reactors are selected depending on the amount of metal or alloyto be processed, mode of heating, extent of heating (temperature)required, and the like. A preferred reactor in the present method is aninduction furnace reactor, which is capable of operating in a frequencyrange of 0 Hz to about 10,000 Hz, 0 Hz to about 3,000 Hz, or 0 Hz toabout 1,000 Hz. Reactors operating at lower frequencies are desirablefor larger metal charges, such that a reactor operating at 0-3,000 Hz isgenerally suitable for 20 pound metal charges and a reactor operating at0-1,000 Hz is generally suitable for 5000 pound metal charges.

Typically, reactors of the present method are lined with a suitablecrucible and appropriately sealed from the external environment enablingvery tight control of the internal chemical environment (e.g., part perthousand, part per million, or the like). Crucibles are selected, inpart, based on the amount of metal or alloy to be heated and thetemperature of the method. Crucibles selected for the present methodtypically have a capacity from about five pounds to about five tons. Onepreferred crucible is comprised of 89.07% Al₂O₃, 10.37% SiO₂, 0.16%TiO₂, 0.15% Fe₂O₃, 0.03% CaO, 0.01% MgO, 0.02% Na₂O₃, and 0.02% K₂O, andhas a 9 inch outside diameter, a 7.75 inch inside diameter, and a 14inch depth. A second preferred crucible is comprised of 99.68% Al₂O₃,0.07% SiO₂, 0.08% Fe₂O₃, 0.04% CaO, and 0.12% Na₂O₃, and has a 4.5 inchoutside diameter, a 3.75 inch inside diameter and a 10 inch depth.

A new composition of matter of the present invention can manifest itselfas a transient, adjustable, or permanent change in energy and/orassociated properties, as broadly defined. Property change can beexhibited as or comprise a change in: (1) structural atomic character(e.g., XES/XRF peak creation, peak fluidity, peak intensity, peakcentroid, peak profile or shape as a function of material/sampleorientation, atomic energy level(s), and TEM, STM, MFM scans); (2)electronic character (e.g., SQUID, scanning SQUID, scanningmagnetoresistive microscopy, scanning magnetic microscope, magnetometer,non-contact MFM, electron electromagnetic interactions, quantum (ortopological) order^(1,2), quantum entanglement³, Jahn-Teller effect,ground state effects, electromagnetic field position/orientation, energygradients, Hall effect, voltage, capacitance, voltage decay rate,voltage gradient, voltage signature including slope of decay and/orchange of slope decay, voltage magnitude, voltage orientation); (3)structural molecular or atomic character (e.g., SEM, TEM, STM, AFM, LFM,and MFM scans, optical microscopy images, and structural orientation,ordering, long range alignment/ordering, anisotropy); (4) physicalconstants (e.g., color, crystalline form, specific rotation, emissivity,melting point, boiling point, density, refractive index, solubility,hardness, surface tension, dielectric, magnetic susceptibility,coefficient of friction, x-ray wavelengths); (5) physical properties(e.g., mechanical, chemical, electrical, thermal, engineering, and thelike); and, (6) other changes that differentiate naturally occurringmaterials from manufactured materials created by inducing a change inmatter.

A preferred analytical method is x-ray fluorescence spectrometry. X-rayfluorescence spectrometry is described in “X-Ray FluorescenceSpectrometry”, by George J. Havrilla in “Handbook of InstrumentalTechniques for Analytical Chemistry,” Frank A. Settle, Ed.,Prentice-Hall, Inc: 1997, which is incorporated herein by reference. XRFspectrometry is a well-known and long-practiced method, which has beenused to detect and quantify or semi-quantify the elemental composition(for elements with Z≧11) of solid and liquid samples. This techniquebenefits from minimal sample preparation, wide dynamic range, and beingnondestructive. Typically, XRF data are not dependent on which dimension(e.g., axial or radial) of a sample was analyzed. Accuracy of less than1% error can generally be achieved with XRF spectrometry, and thetechnique can have detection limits of parts per million.

XRF spectrometry first involves exciting an atom, such that an innershell electron is ejected. Upon ejection of an electron, an outer shellelectron will “drop” down into the lower-energy position of the ejectedinner shell electron. When the outer shell electron “drops” into thelower-energy inner shell, x-ray energy is released. Typically, anelectron is ejected from the K, L, or M shell and is replaced by anelectron from the L, M, or N shell. Because there are numerouscombinations of ejections and replacements possible for any givenelement, x-rays of several energies are emitted during a typical XRFexperiment. Therefore, each element in the Periodic Table has a standardpattern of x-ray emissions after being excited by a sufficientlyenergetic source, since each such element has its own characteristicelectronic state. By matching a pattern of emitted x-ray energies tovalues found in tables, such as those on pages 10-233 to 10-271 of“Handbook of Chemistry and Physics, 73^(rd) Edition,” edited by D. R.Lide, CRC Press, 1992, which is incorporated herein by reference, onecan identify which elements are present in a sample. In addition, theintensity of the emitted x-rays allows one to quantify the amount of anelement in a sample.

There are two standard variations of the XRF technique. First, as anenergy-dispersive method (EDXRF), the XRF technique uses a detector suchas a Si(Li) detector, capable of simultaneously measuring the energy andintensity of x-ray photons from an array of elements. EDXRF iswell-suited for rapid acquisition of data to determine gross elementalcomposition. Typically, the detection limits for EDXRF are in the rangeof tens to hundreds of parts-per-million. A wavelength-dispersivetechnique (WDXRF) is generally better-suited for analyses requiring highaccuracy and precision. WDXRF uses a crystal to disperse emitted x-rays,based on Bragg's Law. Natural crystals, such as lithium fluoride andgermanium, are commonly used for high-energy (short wavelength) x-rays,while synthetic crystals are commonly used for low-energy (longerwavelength) x-rays. Crystals are chosen, in part, to achieve desiredresolution, so that x-rays of different energies are dispersed todistinguishable 2θ angles. WDXRF can either measure x-rays sequentially,such that a WDXRF instrument will step through a range of 2θ angles inrecording a spectrum, or there will be detectors positioned at multiple2θ angles, allowing for more rapid analysis of a sample. Detectors forWDXRF commonly include gas ionization and scintillation detectors. Afurther description of the use of WDXRF technique in the presentinvention can be found in Example 1. Results from EDXRF and results fromWDXRF can be compared by determining the relationship between a 2θ angleand the wavelength of the corresponding x-ray (e.g., using Bragg's Law)and converting the wavelength into energy (e.g., energy equals thereciprocal of the wavelength multiplied by Planck's constant and thevelocity of light).

Analysis of emitted x-rays can be carried out automatically orsemi-automatically, such as by using a software package (e.g., UniQuant,which is sold by Omega Data Systems BV, Veldhoven, The Netherlands) foreither EDXRF or WDXRF. UniQuant is used for standard-less,semi-quantitative to quantitative XRF analysis using the intensitiesmeasured by a sequential x-ray spectrometer. The software packageunifies all types of samples into one analytical program. The UniQuantsoftware program is highly effective for analyzing samples for which nostandards are available. Sample preparation is usually minimal or notrequired at all. Samples can be of very different natures, sizes andshapes. Elements from fluorine or sodium up to uranium, or their oxidecompounds, can be analyzed in samples such as a piece of glass, a screw,metal drillings, lubricating oil, loose fly ash powder, polymers,phosphoric acid, thin layers on a substrate, soil, paint, the year ringsof trees, and, in general, those samples for which no standards areavailable. The reporting is in weight % along with an estimated errorfor each element.

In software packages such as UniQuant, an XRF spectrum is composed ofdata channels. Each data channel corresponds to an energy range andcontains information about the number of x-rays emitted at that energy.The data channels can be combined into one coherent plot to show thenumber or intensity of emitted x-rays versus energy or 2θ angle (the 2θangle is related to the wavelength of an x-ray), such that the plot willshow a series of peaks. An analysis of the peaks by one skilled in theart or the software package can identify the correspondence between theexperimentally-determined peaks and the previously-determined peaks ofindividual elements. For an element, peak location (i.e., the centroidof the peak with respect to energy or 2θ angle), peak profile/shape,peak creation, and peak fluidity would be expected to be essentially thesame, within experimental error, for any sample containing the element.If the same quantity of an element is present in two samples, intensitywill also be essentially the same, excepting experimental error andmatrix effects.

A typical software package is programmed to correlate certain datachannels with the emitted x-rays of elements. Quantification of theintensity of emitted x-rays is accomplished by integrating the XRFspectrum over a number of data channels. Based on the measuredintensities and the previously-compiled data on elements, the softwarepackage will integrate over all data channels, correlate the emittedx-ray intensities, and will then calculate the relative abundance orquantity of elements which appear to be present in a sample, based uponcomparison to the standards. Composition of matter changes produced bythe present invention will generally be characterized by an XRF spectrumthat reports: (1) the presence of an element which was not present inthe starting material and was not added during the process; (2) anincreased amount of an element that was not added to the process in theamount measured; or, (3) a decreased amount of an element that was notremoved during the process in the amount indicated. Examples of (3)include a reduction in identifiable spectra referencing the sum beforenormalization and/or reappearance of an element upon combustion.Products of the present invention can also be characterized by thedifference between XRF Uniquant analysis such as by burning the sample(e.g., LECO analysis), described in more detail below.

A “LECO” analysis is meant to include an analysis conducted by theCS-300 Carbon/Sulfur determinator supplied by a LECO computer. TheCS-300 Carbon/Sulfur determinator is a microprocessor based, softwaredriven instrument for measurement of carbon and sulfur content inmetals, ores, ceramics and other inorganic materials.

Analysis begins by weighing out a sample (1 g nominal) into a ceramiccrucible on a balance. Accelerator material is added, the crucible isplaced on the loading pedestal, and the ANALYZE key is pressed. Furnaceclosure is performed automatically, then the combustion chamber ispurged with oxygen to drive off residual atmospheric gases. Afterpurging, oxygen flow through the system is restored and the inductionfurnace is turned on. The inductive elements of the sample andaccelerator couple with the high frequency field of the furnace. Thepure oxygen environment and the heat generated by this coupling causethe sample to combust. During combustion all elements of the sampleoxidize. Carbon bearing elements are reduced, releasing the carbon,which immediately binds with the oxygen to form CO and CO2, the majoritybeing CO2. Also, sulfur bearing elements are reduced, releasing sulfur,which binds with oxygen to form SO₂.

Sample gases are swept in the carrier stream. Sulfur is measured assulfur dioxide in the first IR cell. A small amount of carbon monoxideis converted to carbon dioxide in the catalytic heater assembly whilesulfur trioxide is removed from the system in a cellulose filter. Carbonis measured as carbon dioxide in the IR cells, as gases flow trough theIR cells.

Ideally, the relative abundances will total 100% prior to normalization.However, for a variety of reasons, such as improper or insufficientcalibration, and/or non-planar sample surface the relative abundanceswill not total 100% prior to normalization. Another reason that therelative abundances of elements do not total 100% prior to normalizationis that a portion of the XRF spectrum falls outside of the data channelsthat the software package correlates with an element (i.e., a portion ofthe XRF spectrum is not recognized as belonging to an element and is notincluded in the relative abundance calculation). In this case, therelative abundances will likely total less than 100% prior tonormalization. Further, the samples will often have anisotropiccharacteristics whereby an axial scan is distinct from a radial scan.Thus, products of the invention may be characterized by an XRF spectrumthat is not recognized by the Uniquant software (e.g., sum of knownconcentrations before normalization is less than 100%) described hereinin an amount, for example, of less than 98%, such as less than 90%, suchas less than 80%. In additional embodiments, the software packagereports or detects one or more elements not detected by other methods orare detected in different quantities.

X-ray emission spectrometry (XES), a technique analogous to XRF, alsoprovides electronic information about elements. In XES, a lower-energysource is used to eject electrons from a sample, such that only thesurface (to several micrometers) of the sample is analyzed. Similar toXRF, a series of peaks is generated, which corresponds to outer shellelectrons replacing ejected inner shell electrons. The peak shape, peakfluidity, peak creation, peak intensity, peak centroid, and peak profileare expected to be essentially the same, within experimental error andmatrix effects, for two samples having the same composition.

Thus, XES analysis of the control standard compared to the atomicallyaltered (i.e., manufactured or tailored) state can also be analyzed.Manufactured copper in the axial direction exhibits similar compositionto natural copper (i.e., 99.98%_(wt)), but radial scans exhibit newpeaks in the region close to naturally occurring S, Cl, and K. Theshifting centroid of the observed peaks from the natural species (i.e.,S, Cl, and K) confirms electronic change in the atomic state of the baseelement. Conventional chemical analysis performed using a LECO (IR)analyzer to detect SO_(x) in the vapor phase post sample combustionconfirmed the absence of sulfur at XES lower detection limits.

Non-contact, magnetic force microscopy image or scanning tunnelingmicroscopy (STM) scan can also confirm the production of a newcomposition of matter or manufactured or tailored material, identifiedby an altered and aligned electromagnetic network. Individually, andfrom differing vantage points, these scans show the outline of thechanged electromagnetic energy network.

New compositions of matter can be electronically modified to induce longrange ordering/alignment. Optical microscopy and SEM imaging of thematerial verifies the degree and extent of long range ordering achieved.

Non-contact, magnetic force microscopy image or scanning tunnelingmicroscopy (STM) scans can also confirm the production of a newcomposition of matter or manufactured or tailored material, identifiedby an altered and aligned electromagnetic network. Individually, andfrom differing vantage points, these scans can show the outline of thechanged electromagnetic energy network. Non-contact MFM imaging can showthat products of the invention often possess clear pattern repetitionand intensity of the manufactured material when compared to the naturalmaterial, or starting material. Products of the invention can becharacterized by the presence of magnetic properties in high purity,non-magnetic metals, such as elemental copper (e.g., 99.98%_(wt)).

Products can also be characterized by color changes. The variation incolor of copper products ranged from black, copper, gold, silver andred. Other visual variations included translucency and near transparencyat regions. While not being bound by theory, the alteration of copper'selectronic state along the continuum enables the new composition ofmatter's color to be adjusted along the continuum.

In several examples of the present invention, the ingots obtained by theprocess possess a substantial internal void and absence of a crown ofmaterial on the top surface. In other examples of the invention, theingot is characterized by essentially no void, with a crown of materialon the top.

Other products of the processes are characterized by changes inhardness. The variation in diamond pyramid hardness between differentmanufactured copper samples ranged from about 25 to 90 (or 3 to 9 timeshigher than natural copper). Hardness change can be anisotropic.

The operations described in the embodiments presented herein did notresult merely from empirical explorations. Rather, guidance was obtainedfrom theoretical considerations regarding the topological aspects ofelectrodynamics. These enabled specification of the range and durationof temperature cycles, the selection of specific combinations andconcentrations of gases to be used, geometric factors affecting thelance placement, and all other chief features of the experimentalprotocols. While not being bound by theory, the Applicant believes theapplication of topological principles^(4,5,6,7,8,9,10) when applied toelectrodynamics provides a powerful means for altering the properties ofmaterials.

As noted in U.S. Ser. No. 09/416,720, the theoretical analysis can beformulated in terms of an allowed set of mathematical poles, defined asthe zurn operator, and further characterized by the set of mathematicalpoles coalesced, defined as the isozurn value. Adjusting or manipulatingthe zurn causes the isozurn value to differ from its starting ornaturally occurring value, thereby modifying the electronic structurefrom that of the natural state.

The products produced by the process have utilities readily apparent tothose skilled in the art. Indeed, materials which comprise metals can beused to manufacture products having adjustable chemical properties(e.g., regioselectivity, regiospecificity, or reaction rate), electronicproperties (e.g., band gap, susceptibility, resistivity, or magnetism),mechanical properties (e.g., ductility or hardness) and/or opticalproperties (e.g., color).

The invention further relates to the apparatus used to produce thematerials. The apparatus of the invention includes a reactor comprisingan induction furnace characterized by a gas source and at least oneradiation source arranged to expose the gas and/or the contents of thereactor, in the manner discussed above, optional filters and optionalenvironmental controls. As such, the invention includes an apparatuscomprising a combination of the following: (a) a first and a secondpencil lamp; (b) at least one short arc lamp within a housing; (c) a gassource proximal to (b) and an induction furnace.

In one embodiment, the radiation source is proximate to a gas sourcewhich is adapted to control the environment of the radiation source. Inanother embodiment, the short arc lamp housing further comprises atleast one pencil lamp, such as those discussed above. In anotherembodiment, the apparatus further comprises a filter, such as thosedescribed herein.

Exemplification Example 1 Experimental Procedure for Copper Method “AB”Run 14-03-02

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100 pound induction furnace reactor (Inductotherm)fitted with a 73-30R Powertrak power supply was charged with 9080 gcopper (99.98% purity) through its charging port. Prior to charging agas addition lance was placed inside the reactor at the reactorcenterline and placed two inches from the bottom of the bath. Thereactor was fitted with a graphite cap and a ceramic liner (i.e., thecrucible, from Engineering Ceramics). During the entire procedure, aslight positive pressure of 97% argon and 3% hydrogen (˜0.5 psig) wasmaintained in the reactor using a continuous backspace purge. Thereactor was heated to the metal charge liquidus point plus at least 300°F., at a rate no greater than 300° F./hr, as limited by the integrity ofthe crucible. The induction furnace operated in the frequency range of 0Hz to 3000 Hz, with frequency determined by a temperature-controlledfeedback loop implementing an Omega Model CN3000 temperature controller.The temperature was increased to 2462° F. again using a rate no greaterthan 300° F./hour. When this temperature was reached, graphitesaturation assemblies (⅜ inches OD, 36 inches long high purity (<5 ppmimpurities) graphite rods) were inserted to the bottom of the coppercharge through ports located in the top plate. The copper was held at2462° F. for 2 hours. Every 30 minutes during the hold period, anattempt was made to lower the graphite saturation assemblies asdissolution occurred. As the copper became saturated with carbon, thegraphite saturation assemblies were consumed. After the 2-hour holdperiod was complete, the graphite saturation assemblies were removed.

The reactor temperature was increased to 2515° F. over 7 minutes. Thetemperature was then varied between 2476° F. and 2515° F. for 16.5cycles. Each cycle consisted of raising the temperature continuouslyover 7 minutes and lowering the temperature continuously over 7 minutes.After the 15 cycles were completed, the gas flow rate was started in abypass mode at a rate of 0.3 L/min of 97% argon and 3% neon (all gascompositions are constant unless stated otherwise). Five minutes intothe 15.5^(th) cycle, a xenon radiation source is activated within thesealed enclosure. At 6 minutes into the 15.5^(th) cycle, a long waveultraviolet radiation source was activated in the sealed enclosure. Atsweep count 15.5, the gas flow was redirected to direct bath addition.At sweep count 16, a short wave ultraviolet radiation source wasinitiated in the sealed enclosure. At sweep count 16.5, the xenonradiation source was remotely rotated within the sealed enclosure. Thetemperature of the copper was varied over another 5 cycles between 2476°F. and 2515° F. After the fifth cycle, the reactor temperature waslowered to 2462° F. over a 10-minute period.

The graphite saturation assemblies were reinstalled in the copper andremained there for 1 hour. The graphite saturation assemblies wereremoved. The reactor temperature was lowered to 2459° F. over 5 minutes.The reactor was held at this temperature for 5 minutes with continuedgas addition. The temperature was then varied between 2453° F. and 2459°F. over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. After the 20^(th) cycle, third body addition (gasaddition) was changed to a flow rate of 9 mL/min of 100% neon. The bathwas then cooled to 2450° F. over 10 minutes.

The temperature was then varied between 2441° F. and 2450° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 0.15 L/min flow of 40%helium, 60% argon and trace neon was added, and while lowering thetemperature, a 0.3 L/min flow of 40% argon, 60% helium, trace neon,trace hydrogen, and trace krypton was added. After the 4.5 cycles, theshort wave radiation source within the sealed enclosure was terminated.The reactor temperature was then lowered to 2438° F. over 1 minute. Thetemperature was varied between 2406° F. and 2438° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 0.15 L/min flow of 40%helium, 60% argon and trace neon was added, and while lowering thetemperature, a 0.3 L/min flow of 40% argon, 60% helium, trace neon,trace hydrogen, and trace krypton was added. After the final cycle(sweep), gas flow was changed to trace neon only.

The temperature was then varied between 2419° F. and 2406° F. for onecycle. The cycle consisted of raising the temperature continuously over15 minutes and lowering the temperature continuously over 15 minutes. Atthe completion of this temperature sweep, the reactor temperature waslowered to T_(solidus) plus 11° F. over 45 minutes.

Upon reaching T_(solidus) plus 11° F., gas addition was changed to 0.3L/min of 100% hydrogen and trace neon and held for five minutes. Thereactor was then cooled to T_(solidus) plus 10° F. over five minutes.Upon reaching T_(solidus) plus 10° F., the gas addition lance wasrelocated into the headspace of the reactor, such that a quarter inch (¼inches) dimple could be observed on the bath surface. The bath was heldat T_(solidus) plus 10° F. for an additional 5 minutes for conditioningand equilibrization. The reactor was then cooled to T_(solidus) plus 8°F. while maintaining a temperature lowering rate of no more than 3°F./hr. Upon reaching T_(solidus) plus 8° F. a manual power pulse of 2 kWwas introduced with a single continuous up/down sweep from normalholding power. The reactor was then cooled to T_(solidus) plus 2° F.while maintaining a temperature lowering rate of no more than 3° F./hr.Upon reaching T_(solidus) plus 2° F. a manual power pulse of 1.5 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. Furthermore, immediately following the manual power pulse the gasflow rate was changed to 0.15 L/min of 49.5% hydrogen, 49.5% helium and1% neon. The reactor was then cooled to T_(solidus) again maintaining atemperature-lowering rate of no more than 3° F./hr. Upon reachingT_(solidus), the reactor temperature was lowered to T_(solidus) minus75° F. over five hours. Upon reaching T_(solidus) minus 75° F., the flowrate was changed to 30 ml/min of 60% helium, 40% hydrogen and traceneon. The induction furnace power supply was then lowered to 0.75 kW andthe reactor was allowed to cool to 1000° F. Upon reaching 1000° F., theflow rate was changed to 30 m/min of 100% helium and trace neon. Theinduction furnace power supply was lowered to 0.50 kW and the reactorwas allowed to cool to 350° F. Upon reaching 350° F., the inductionfurnace power supply was shut down. A timer was initiated. At a time of5 minutes, the long wave radiation source within the sealed enclosurewas terminated. At a time of 9 minutes, the xenon radiation sourcewithin the sealed enclosure was terminated. At a time of 15 minutes, thetrace neon gas addition was terminated. At a time of 30 minutes, thehelium gas addition was terminated. At a time of 45 minutes, the ingotand crucible were removed from the reactor in the presence of radiationsources (metal halide light sources) utilizing tongs.

Upon removal, the crucible was stripped from the metal ingot via agentle wedging action. Immediately following removal, the ingot wastransferred into a quench chamber containing water, ensuring that thetop of the ingot surface was covered by at least 6 inches of water. Theingot was allowed to stay in the quench vessel for 6 hours prior to itsremoval from the quench vessel. Note: An identical experimental programexcept for the use of pencil lamps—which provided a source ofelectromagnetic radiation to the third-body gases—was also performedverifying the efficacy of the improved process (See 14-03-03 in Table 1and attending discussions).

Example 2 Experimental Procedure for Copper Method “HA” Run 14-02-06

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100 pound induction furnace reactor (Inductortherm)fitted with a 73-30R Powertrak power supply was charged with 9080 gcopper (99.98% purity) through its charging port. The reactor was fittedwith a graphite cap and a ceramic liner (i.e., the crucible, fromEngineering Ceramics). During the entire procedure, a slight positivepressure of nitrogen (˜0.5 psig) was maintained in the reactor using acontinuous backspace purge. The reactor was heated to the metal chargeliquidus point plus at least 300° F., at a rate no greater than 300°F./hr, as limited by the integrity of the crucible. The inductionfurnace operated in the frequency range of 0 Hz to 3000 Hz, withfrequency determined by a temperature-controlled feedback loopimplementing an Omega Model CN3000 temperature controller. Thetemperature was increased to 2462° F. again using a rate no greater than300° F./hour. When this temperature was reached, graphite saturationassemblies (⅜ inch OD, 36 inch long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the copper charge throughports located in the top plate. The copper was held at 2462° F. for 2hours. Every 30 minutes during the hold period, an attempt was made tolower the graphite saturation assemblies as dissolution occurred. As thecopper became saturated with carbon, the graphite saturation assemblieswere consumed. After the 2 hour hold period was complete, the graphitesaturation assemblies were removed.

The reactor temperature was increased to 2539° F. over 14 minutes. Atthis point, a gas addition lance was lowered into the molten metal to aposition approximately 2 inches from the bottom of the reactor and a 4.8L/min flow of gas was begun. The gas composition was 92% argon, 3% neon,and 5% helium. The temperature was then lowered to 2515° F. over 10minutes. Flow rate was then lowered to 2.4 L/min with the same ratio ofgases (argon, neon, and helium). The temperature was then varied between2476° F. and 2515° F. for 15 cycles. Each cycle consisted of raising thetemperature continuously over 7 minutes and lowering the temperaturecontinuously over 7 minutes. After the 15 cycles were completed, the gasflow rate was altered again to 1.4 L/min (all gas compositions areconstant unless stated otherwise). The temperature of the copper wasvaried over another 5 cycles between 2476° F. and 2515° F. After thefifth cycle, the reactor temperature was lowered to 2462° F. over a 30minute period with a lowered gas addition rate of 0.8 L/min.

The graphite saturation assemblies were reinstalled in the copper andremained there for 1 hour. The graphite saturation assemblies wereremoved. Flow rate was increased to 1.2 L/min. The reactor temperaturewas lowered to 2459° F. over 5 minutes. The reactor was held at thistemperature for 5 minutes with continued gas addition. The temperaturewas then varied between 2453° F. and 2459° F. over 20 cycles. Each cycleconsisted of lowering the temperature continuously over 9 minutes andraising the temperature continuously over 9 minutes. During thetemperature lowering portion of the cycle, gas addition was at the rateof 1.4 L/min with a gas composition of 95% argon, 3% neon, 2% krypton.During the temperature increasing portion of the cycle, gas addition wasat the rate of 2.8 L/min with a gas composition of 95% argon, 5% neon.After the 20^(th) cycle, third body addition (gas addition) was changedto a flow rate of 0.15 L/min with a gas composition of 95% helium, 5%krypton. The bath was then cooled to 2450° F. over 13 minutes.

The temperature was then varied between 2441° F. and 2450° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 1.2 L/min flow of 95%helium, 5% krypton was added, and while lowering the temperature, a 2.4L/min flow of 95% argon, 5% neon was added. After the 4.5 cycles, thereactor temperature was lowered to 2438° F. over 1 minute. Thetemperature was varied between 2406° F. and 2438° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 1.2 L/min flow of 95%nitrogen, 5% helium was added, and while lowering the temperature, a 2.4L/min flow of 95% argon, 5% neon was added. After the final cycle(sweep), gas flow was changed to 0.15 L/min with a gas composition of95% helium, 5% argon. The reactor was then held for 16 minutes at 2406°F.

The temperature was then varied between 2419° F. and 2406° F. for onecycle. The cycle consisted of raising the temperature continuously over15 minutes and lowering the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 2.4 L/min flow of 95% helium,5% argon was added, and while lowering the temperature, a 1.2 L/min flowof 95% argon, 5% nitrogen was added. At the completion of thistemperature sweep, the reactor temperature was lowered to T_(solidus)plus 10° F.

The gas addition lance was relocated into the headspace of the reactor,such that a quarter inch (¼ inches) dimple could be observed on the bathsurface (1.2 L/min flow of 95% argon, 5% nitrogen). The bath was held atT_(solidus) plus 10° F. for an additional 5 minutes for conditioning andequilibrization. The reactor was then cooled to T_(solidus) plus 8° F.while maintaining a temperature lowering rate of no more than 3° F./hr.Upon reaching T_(solidus) plus 8° F. a manual power pulse of 2 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. The reactor was then cooled to T_(solidus) plus 2° F. whilemaintaining a temperature lowering rate of no more than 3° F./hr. Uponreaching T_(solidus) plus 2° F. a manual power pulse of 1.5 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. The reactor was then cooled to T_(solidus) again maintaining atemperature lowering rate of no more than 3° F./hr. Upon reachingT_(solidus), the induction furnace power supply was lowered to 1 kW andthe reactor was allowed to cool from T_(solidus) to T_(solidus) minus20° F. Upon reaching T_(solidus) minus 20° F., the induction furnacepower supply was lowered to 0.75 kW and the reactor was allowed to coolto 1000° F. Upon reaching 1000° F., the induction furnace power supplywas lowered to 0.50 kW and the reactor was allowed to cool to 350° F.Immediately after setting the power to 0.5 kW, the gas flow rate waschanged to 0.15 L/min with a gas composition of 95% argon, 5% nitrogen.Upon reaching 350° F., the induction furnace power supply was shut down.Thirty minutes were allowed to pass. The ingot and crucible were removedfrom the reactor using titanium metal tongs in the presence of lightsupplied by metal halide ceiling lamps.

Upon removal, the crucible was stripped from the metal ingot via agentle wedging action. Immediately following removal, the ingot wastransferred into a quench chamber containing deionized water, ensuringthat the top of the ingot surface was covered by at least 6 inches of DIwater. Upon entrance into the quench chamber, a timer was established.At a time of 10 hours and 30 minutes, the ingot was removed from thequench system using the titanium metal tongs and transferred to a cleansurface. Exposure to external radiation sources included the metalhalide light and placement directly under a skylight (which addedfiltered sunlight to the irradiation sources). The timer was then resetto zero. The ingot was irradiated for 10 minutes at which point anadditional radiation source (krypton lamp) was initiated. At 18 minutes,two orthogonal fluorescent lamp racks were turned on. At 30 minutes, twoangled metal halide lights were simultaneously turned on. At this pointthe timer was again reset. At a time of 6 hours, the krypton lamp, twoorthogonal fluorescent lamp racks, and the two angled metal halidelights were sequentially turned off. The timer was again reset to zero.At a time of 6 hours, 30 minutes, normal lab lighting (metal halides)was turned off. The timer was reset to zero. For 48 hours, the ingot wasallowed to stabilize with no manual intervention (i.e., no handling).

Example 3 Experimental Procedure for Aluminium Method “HA” Run 14-04-02

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100 pound induction furnace reactor (Inductortherm)fitted with a 73-30R Powertrak power supply was charged with 4540 gAluminum (99.99% purity) through its charging port. The reactor wasfitted with a graphite cap and a ceramic liner (i.e., the crucible, fromEngineering Ceramics). During the entire procedure, a slight positivepressure of nitrogen (˜0.5 psig) was maintained in the reactor using acontinuous backspace purge. The reactor was heated to the metal chargeliquidus point plus at least 300° F., at a rate no greater than 300°F./hr, as limited by the integrity of the crucible. The inductionfurnace operated in the frequency range of 0 Hz to 3000 Hz, withfrequency determined by a temperature-controlled feedback loopimplementing an Omega Model CN3000 temperature controller. Thetemperature was increased to 1650° F. again using a rate no greater than300° F./hour. When this temperature was reached, graphite saturationassemblies (⅜ inch OD, 36 inch long high purity (<5 ppm impurities)graphite rods) were inserted to the bottom of the aluminum chargethrough ports located in the top plate. The aluminum was held at 1650°F. for 2 hours. Every 30 minutes during the hold period, an attempt wasmade to lower the graphite saturation assemblies as dissolutionoccurred. As the aluminum became saturated with carbon, the graphitesaturation assemblies were consumed. After the 2 hour hold period wascomplete, the graphite saturation assemblies were removed.

The reactor temperature was increased to 1690° F. over 14 minutes. Atthis point, a gas addition lance was lowered into the molten metal to aposition approximately 2 inches from the bottom of the reactor and a 4.8L/min flow of gas was begun. The gas composition was 92% argon, 3% neon,and 5% helium. The temperature was then lowered to 1678° F. over 10minutes. Flow rate was then lowered to 2.4 L/min with the same ratio ofgases (argon, neon, and helium). The temperature was then varied between1657° F. and 1678° F. for 15 cycles. Each cycle consisted of raising thetemperature continuously over 7 minutes and lowering the temperaturecontinuously over 7 minutes. After the 15 cycles were completed, the gasflow rate was altered again to 1.4 L/min (all gas compositions areconstant unless stated otherwise). The temperature of the aluminum wasvaried over another 5 cycles between 1657° F. and 1678° F. After thefifth cycle, the reactor temperature was lowered to 1650° F. over a 30minute period with a lowered gas addition rate of 0.8 L/min.

The graphite saturation assemblies were reinstalled in the aluminum andremained there for 1 hour. The graphite saturation assemblies wereremoved. Flow rate was increased to 1.2 L/min. The reactor temperaturewas lowered to 1648° F. over 5 minutes. The reactor was held at thistemperature for 5 minutes with continued gas addition. The temperaturewas then varied between 1646° F. and 1644° F. over 20 cycles. Each cycleconsisted of lowering the temperature continuously over 9 minutes andraising the temperature continuously over 9 minutes. During thetemperature lowering portion of the cycle, gas addition was at the rateof 1.4 L/min with a gas composition of 95% argon, 3% neon, 2% krypton.During the temperature increasing portion of the cycle, gas addition wasat the rate of 2.8 L/min with a gas composition of 95% argon, 5% neon.After the 20^(th) cycle, third body addition (gas addition) was changedto a flow rate of 0.15 L/min with a gas composition of 95% helium, 5%krypton. The bath was then cooled to 1643° F. over 13 minutes.

The temperature was then varied between 1639° F. and 1643° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 1.2 L/min flow of 95%helium, 5% krypton was added, and while lowering the temperature, a 2.4L/min flow of 95% argon, 5% neon was added. After the 4.5 cycles, thereactor temperature was lowered to 1637° F. over 1 minute. Thetemperature was varied between 1620° F. and 1637° F. for 15.5 cycles.Each cycle consisted of lowering the temperature continuously over 15minutes and raising the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 1.2 L/min flow of 95%nitrogen, 5% helium was added, and while lowering the temperature, a 2.4L/min flow of 95% argon, 5% neon was added. After the final cycle(sweep), gas flow was changed to 0.15 L/min with a gas composition of95% helium, 5% argon. The reactor was then held for 16 minutes at 1620°F.

The temperature was then varied between 1627° F. and 1620° F. for onecycle. The cycle consisted of raising the temperature continuously over15 minutes and lowering the temperature continuously over 15 minutes. Inaddition, while raising the temperature, a 2.4 L/min flow of 95% helium,5% argon was added, and while lowering the temperature, a 1.2 L/min flowof 95% argon, 5% nitrogen was added. At the completion of thistemperature sweep, the reactor temperature was lowered to T_(solidus)plus 10° F.

The gas addition lance was relocated into the headspace of the reactor,such that a quarter inch (¼ inches) dimple could be observed on the bathsurface (1.2 L/min flow of 95% argon, 5% nitrogen). The bath was held atT_(solidus) plus 10° F. for an additional 5 minutes for conditioning andequilibration. The reactor was then cooled to T_(solidus) plus 8° F.while maintaining a temperature lowering rate of no more than 3° F./hr.Upon reaching T_(solidus) plus 8° F. a manual power pulse of 2 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. The reactor was then cooled to T_(solidus) plus 2° F. whilemaintaining a temperature lowering rate of no more than 3° F./hr. Uponreaching T_(solidus) plus 2° F. a manual power pulse of 1.5 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. The reactor was then cooled to T_(solidus) again maintaining atemperature lowering rate of no more than 3° F./hr. Upon reachingT_(solidus) the induction furnace power supply was lowered to 1 kW andthe reactor was allowed to cool from T_(solidus) to T_(solidus) minus20° F. Upon reaching T_(solidus) minus 20° F., the induction furnacepower supply was lowered to 0.75 kW and the reactor was allowed to coolto 1000° F. Upon reaching 1000° F., the induction furnace power supplywas lowered to 0.50 kW and the reactor was allowed to cool to 350° F.Immediately after setting the power to 0.5 kW, the gas flow rate waschanged to 0.15 L/min with a gas composition of 95% argon, 5% nitrogen.Upon reaching 350° F., the induction furnace power supply was shut down.Thirty minutes were allowed to pass. The ingot and crucible were removedfrom the reactor using titanium metal tongs in the presence of lightsupplied by metal halide ceiling lamps.

Upon removal, the crucible was stripped from the metal ingot via agentle wedging action. Immediately following removal, the ingot wastransferred into a quench chamber containing deionized water, ensuringthat the top of the ingot surface was covered by at least 6 inches of DIwater. Upon entrance into the quench chamber, a timer was established.At a time of 10 hours and 30 minutes, the ingot was removed from thequench system using the titanium metal tongs and transferred to a cleansurface. Exposure to external radiation sources included the metalhalide light and placement directly under a skylight (which addedfiltered sunlight to the irradiation sources). The timer was then resetto zero. The ingot was irradiated for 10 minutes at which point anadditional radiation source (krypton lamp) was initiated. At 18 minutes,two orthogonal fluorescent lamp racks were turned on. At 30 minutes, twoangled metal halide lights were simultaneously turned on. At this pointthe timer was again reset. At a time of 6 hours, the krypton lamp, twoorthogonal fluorescent lamp racks, and the two angled metal halidelights were sequentially turned off. The timer was again reset to zero.At a time of 6 hours, 30 minutes, normal lab lighting (metal halides)was turned off. The timer was reset to zero. For 48 hours, the ingot wasallowed to stabilize with no manual intervention (i.e., no handling).

Example 4 Experimental Procedure for Cobalt, Vanadium, Rhenium Method“HD” RUN 14-01-20

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100 pound induction furnace reactor (Inductotherm)fitted with a 73-30R Powertrak power supply. A gas addition lance wasinstalled to a position approximately ¼ inches from the bottom of thereactor. The reactor was charged with 8899 g cobalt (99.5% purity), 182g vanadium (99.5% purity) and 7 g rhenium (99.997% purity) through itscharging port. The reactor was fitted with a graphite cap and a ceramicliner (i.e., the crucible, from Engineering Ceramics). During the entireprocedure, a slight positive pressure of 97% argon, 3% hydrogen (˜0.5psig) was maintained in the reactor using a continuous backspace purge.Bypass injection of gas addition was commenced (i.e., gas flow divertedaround the reactor was initiated) at a rate of 0.15 L/min of argon. Theincoming gas line for the gas addition lance passes through a sealed,light-tight enclosure whereby irradiation of the gas with preciseradiation sources (e.g., wavelength, intensity, etc) could be achieved.When the entire gas line had been completely purged (assuming a plugflow model), a neon radiation source was activated within the sealedenclosure. A timer was set to zero. Bypass flow was adjusted to 100%argon at a flow rate of 0.15 L/min with trace neon present. (trace canbe defined as ≦0.005% vol. to ≦5%). At a time of 3 minutes, an argonradiation source was activated within the sealed enclosure. Aftercompletion of another gas line purge (assuming a plug flow model), thegas line was switched from bypass to direct injection through the gasaddition lance.

The induction furnace power was then initiated. The reactor was heatedto 450° F., at a rate no greater than 300° F./hr, as limited by theintegrity of the crucible. The induction furnace operated in thefrequency range of 0 Hz to 3000 Hz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN3000temperature controller. Upon reaching 450° F., the gas addition lancewas repositioned to 2 inches from the bottom of the reactor. The timerwas again set to zero. At a time of 2 minutes, the gas composition waschanged to 0.15 L/min of 66% nitrogen, 34% hydrogen with trace neonpresent. After completion of another gas line purge (assuming a plugflow model), a krypton radiation source was initiated in the sealedenclosure. Continue reactor heat up at a rate no greater than 300°F./hr, as limited by the integrity of the crucible, until T_(solidus)minus 30° F. was achieved. The gas flow rate was then increased to 0.3L/min with a constant gas composition. At T_(solidus) a second argonradiation source was activated within the sealed enclosure. ApproachT_(solidus) plus 8° F. over a 3 to 5 minute time span. From T_(solidus)plus 8° F. to T_(solidus) plus 15° F., reduce the gas flow rate to 0.15L/min with a constant gas composition. Immediately upon reachingT_(solidus) plus 15° F., a second neon radiation source was initiated inthe sealed enclosure. Immediately after the second neon radiation sourcewas initiated, the gas composition was adjusted to 75% hydrogen, 22%nitrogen, 3% argon and trace neon. The molten bath was held at thiscondition for 5 minute for stabilization.

After the 5 minute hold, the gas composition was adjusted to 20% helium,63% nitrogen, 17% argon, and trace neon. The bath was held under theseconditions for an additional 15 minutes. Again, following the hold, thegas composition and flow rate were adjusted to 100% argon with traceneon at a rate of 0.3 L/min. The reactor was held at this condition for3 minutes. The timer was reset to zero. At a time of 65 minutes,graphite saturation assemblies (⅜ inches OD, 36 inches long high purity(<5 ppm impurities) graphite rods) were inserted to the bottom of thecobalt alloy charge through ports located in the top plate. The cobaltwas heated to 2504° F. over a one hour period. The bath was then held atthis condition for 2 hours. Every 30 minutes during the hold period, anattempt was made to lower the graphite saturation assemblies asdissolution occurred. As the cobalt became saturated with carbon, thegraphite saturation assemblies were consumed. After the 2 hour holdperiod was complete, the graphite saturation assemblies were removed. Anadditional 47 grams of graphite powder was charged into the reactorthrough the charging port. The bath was then heated to 3194° F. overthree hours. Upon achieving 3194° F., the gas composition and flow ratewere adjusted to 100% nitrogen with trace neon at a rate of 0.3 L/min.Hold reactor conditions for five minutes. Reduce the gas flow rate to0.15 L/min with constant composition. Immediately following thisreduction in gas flow, the krypton radiation source in the sealedenclosure was turned off. The timer was reset to zero. At a time of 3minutes, the gas flow rate was reduced to 37.5 ml/min with constantcomposition. One of the argon radiation sources inside the sealedenclosure was turned off. At a time of 5 minutes, the nitrogen componentof the gas flow was discontinued, while maintaining the flow of traceneon. At a time of 10 minutes, remotely rotate one of the neon radiationsources within the sealed enclosure. The reactor temperature was loweredto 3064° F. over 7 minutes.

The temperature was then varied between 2851° F. and 3064° F. for 16cycles. Each cycle consisted of raising the temperature continuouslyover 7 minutes and lowering the temperature continuously over 7 minutes.After completion of the 14.5 cycles, argon was reintroduced at a flowrate of 0.15 L/min with trace neon. Five minutes into the 15^(th) cycle,a xenon radiation source was activated within the sealed enclosure. At 6minutes into the 15^(th) cycle, a long wave ultraviolet radiation sourcewas activated in the sealed enclosure. At sweep count 15.5, a short waveultraviolet radiation source was initiated in the sealed enclosure. Atsweep count 16, remotely rotate the xenon radiation source within thesealed enclosure. The temperature of the cobalt was varied over another5 cycles between 2851° F. and 3064° F. After the fifth cycle, thereactor temperature was lowered to 2775° F. over a 10 minute period.Upon achieving the target temperature of 2775, the graphite saturationassemblies were reinstalled in the cobalt and remained there for 1 hour.The graphite saturation assemblies were then removed.

Two voltage probes (source and ground probe) were then installed in theheadspace of the reactor and allowed to equilibrate for 5 minutes. Uponcompletion of the five minute hold the voltage probes were lowered intothe bath. The source probe should be positioned 2 inches below the axialcenter and 1 inch from the radial center. The ground probe waspositioned 0.75 inches above the axial position of the source probe and1 inch from the radial center (180° from the source probe). Once theprobes are installed a five minute hold at this condition is done toallow the bath to electronically equilibrate with the probes. Voltagewas then applied to the probes and varied between multiple voltage setpoints. This voltage application was in a continuous up/down sweepbetween two predetermined voltages. The first voltage cycle was variedbetween 17 and 18 volts for 24 cycles. Each cycle consisted of raisingthe voltage continuously over 45 seconds and lowering the voltagecontinuously over 45 seconds. The second voltage cycle was variedbetween 13.25 and 14.75 volts for 20 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The third voltage cycle was variedbetween 8.75 and 10.25 volts for 17 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The fourth voltage cycle wasvaried between 4.00 and 7.00 volts for 14 cycles. Each cycle consistedof raising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The fifth voltage cycle was variedbetween 1.50 and 5.00 volts for 10 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The sixth voltage cycle was variedbetween 0.50 and 2.00 volts for 3 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. When the final cycle was completedthe voltage was set onto a constant 1 volt setting. This voltageremained constant until a later step during which the leads wereremoved.

The reactor temperature was then lowered to 2759° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued gasaddition. The temperature was then varied between 2727° F. and 2759° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. After the 20^(th) cycle, third body gas addition waschanged by turning off the argon component of the gas leaving only traceneon gas flow. The bath was then cooled to 2711° F. over 5 minutes. Uponreaching 2711° F., one of the neon radiation sources within the sealedenclosure was remotely rotated.

The temperature was then varied between 2662° F. and 2711° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 0.15 L/min flow of 60%argon, 40% helium, and trace neon was added, and while lowering thetemperature, a 0.3 L/min flow of 100% helium, trace neon, and tracekrypton was added. At sweep count 0.5, a krypton radiation source wasinitiated in the sealed enclosure. At sweep count 1.0, an argonradiation source was initiated in the sealed enclosure. At sweep count4.5, the short wave ultraviolet radiation source was terminated in thesealed enclosure. The reactor temperature was lowered to 2645° F. over 5minutes. The temperature was varied between 2467° F. and 2645° F. for15.5 cycles. Each cycle consisted of lowering the temperaturecontinuously over 15 minutes and raising the temperature continuouslyover 15 minutes. In addition, while raising the temperature, a 0.15L/min flow of 60% argon, 40% helium, and trace neon was added, and whilelowering the temperature, a 0.3 L/min flow of 100% helium, trace neon,and trace krypton was added. After the 15.5^(th) cycle, third body gasaddition was changed by turning off all gas components except the traceneon gas flow.

After the 15.5^(th) cycle, a timer was established. At a time of 3minutes, the xenon radiation source within the sealed enclosure wasremotely rotated. The timer was then reset to zero. At 60 minutes, flowrates were adjusted to 0.3 L/min of 100% argon and trace neon. At 65minutes, flow rates were adjusted to 3.0 ml/min of 60% argon, 40%helium, and trace neon. Immediately after the flow was adjusted, one ofthe neon radiation sources within the sealed enclosure was remotelyrotated. At 68 minutes, flow rates were adjusted to 0.15 L/min of 100%helium, trace neon and trace krypton. At 68 minutes 20 seconds, the 1volt power was brought to zero output and the voltage power leadsremoved from the voltage probes. At 68 minutes 30 seconds, the long waveultraviolet radiation source was turned off in the sealed enclosure. At71 minutes 15 seconds, the voltage probes were repositioned to threeinches above the bath surface. At 75 minutes, the source and groundprobe were completely removed from the reactor.

After the voltage probes had been removed from the reactor, flow rateswere adjusted to 0.15 L/min of 77% argon, 18% nitrogen, 5% helium andtrace neon. The reactor was then held at temperature and flow rate for15 minutes. After the 15 minute hold, an argon radiation source wasturned off in the sealed enclosure. The flow rates were immediatelyreadjusted to 0.15 L/min of 77% argon, 12% nitrogen, 11% helium andtrace neon. The reactor was then held at temperature and flow rate for25 minutes. After the 25 minute hold, the krypton radiation source wasturned off in the sealed enclosure. The flow rates were immediatelyreadjusted to 0.30 L/min of 10% argon, 90% helium and trace neon. Thereactor was then held at temperature and flow rate for 3 minutes. Afterthe 3 minute hold, flow rates were adjusted to 0.15 L/min of 10% argon,90% helium and trace neon and held for 2 minutes. After the 2 minutehold, flow rates were adjusted to 0.30 L/min of 7% hydrogen, 93%nitrogen and trace neon and held for 10 minutes. After the 10 minutehold, flow rates were adjusted to 0.15 L/min of 7% hydrogen, 93%nitrogen and trace neon and held for 3 minutes. After the 3 minute hold,flow rates were adjusted to 30 ml/min of 7% hydrogen, 93% nitrogen andtrace neon and held for 2 minutes. After the 2 minute hold, flow rateswere adjusted to 0.15 L/min of 87% argon, 10% nitrogen, 3% helium andtrace neon and held for 5 minutes. After the 5 minute hold, flow rateswere adjusted to 0.6 L/min of 90% argon, 10% nitrogen and trace neon andheld for 7 minutes. After the 7 minute hold, flow rates were adjusted to30 ml/min of 90% argon, 10% nitrogen and trace neon and held for 2minutes. After the 2 minute hold, flow rates were adjusted to 0.60 L/minof 95% argon, 5% nitrogen and trace neon and held for 15 minutes. Afterthe 15 minute hold, flow rates were adjusted to 0.30 L/min of 95% argon,5% nitrogen and trace neon and held for 5 minutes.

The reactor temperature was then lowered to 2541° F. over 21 minutes.The temperature was then varied between 2467° F. and 2541° F. for threecycles. The cycles consisted of raising the temperature continuouslyover 27 minutes and lowering the temperature continuously over 27minutes. After the third cycle, the bath was held at 2541° F. for 5minutes. The reactor temperature was then lowered to 2467° F. over 2minutes 30 seconds. The temperature was then varied between 2541° F. and2467° F. for two cycles. The cycles consisted of raising the temperaturecontinuously over 11 minutes and lowering the temperature continuouslyover 7 minutes.

After the completion of the 2^(nd) cycle, the induction power supply wasplaced into manual control. The power was then instantaneously increased5 kW above the steady state power level and immediately upon hitting the5 kW increase the power was instantaneously decreased back to the steadystate power level. The power level was then varied up 3.7 kW and down3.7 kW over 6 cycles. The cycles consisted of raising power 3.7 kW abovethe steady state power level over 25 seconds. Once raised, the powerlevel was held at the additional 3.7 kW setting for 45 seconds.Following the 45 second hold, the power was lowered back to the steadystate power level over a 15 second time frame.

After the 6^(th) power cycle, the gas flows were adjusted to 0.60 L/minof 100% argon and trace neon and held for 7 minutes. Following the sevenminute hold, the argon flow was secured leaving only the trace neonflow. Once the argon flow was secured, a second lance was positionedinside the reactor. This lance was placed at a distance ⅔ from theradial center and 1.5 inches from the bottom of the bath. The centerlinelance was then repositioned to ¼ inch from the bottom. Once thecenterline lance was repositioned, flow was started in theoff-centerline lance at a rate of 30 ml/min of 100% argon and traceneon. A timer was initiated. At a time of 2 minutes, the trace neon flowin the centerline lance was secured. At a time of 2 minutes 30 seconds,flow was initiated in the centerline lance at a flow rate of 30 ml/minof 100% carbon monoxide and held for 3 minutes. After the 3 minute hold,flow rates were adjusted in the off-centerline lance to 0.15 L/min of100% argon and trace neon and held for 15 minutes. After the 15 minutehold, flow rates were adjusted in the off-centerline lance to trace neononly. Furthermore, the flow rate was adjusted in the centerline lance to0.60 L/min of 100% carbon monoxide and held for 10 minutes. After the 10minute hold, the carbon monoxide in the centerline lance was secured.The reactor temperature was then lowered to T_(solidus) plus 18° F. over30 minutes. Upon reaching the T_(solidus) plus 18° F., flow was adjustedin the centerline lance to 0.30 L/min of 100% carbon monoxide and heldfor 20 minutes. After the 20 minute hold, all flow was secured in thecenterline lance and the lance was removed.

After the centerline lance was removed, adjust flow rates in theoff-centerline lance to 30 ml/min of 88% argon, 12% nitrogen and traceneon, and held for 3 minutes. After the 3 minute hold, flow rates wereadjusted to 0.30 L/min of 25% helium, 75% argon and trace neon and heldfor 10 minutes. After the 10 minute hold, flow rates were adjusted to0.30 L/min of 88% argon, 12% nitrogen and trace neon and held for 10minutes. After the 10 minute hold, flow rates were adjusted to 0.15L/min of 88% argon, 12% nitrogen and trace neon and held for 5 minutes.After the 5 minute hold, flow rates were adjusted to 30 ml/min of 88%argon, 12% nitrogen and trace neon and held for 2 minutes. After the 2minute hold, flow rates were adjusted to 0.15 L/min of 88% argon, 12%nitrogen and trace neon. Once the flow rates were adjusted, the reactortemperature was lowered to T_(solidus) plus 15° F. over 45 minutes. Uponreaching the T_(solidus) plus 15° F., flow was adjusted in theoff-centerline lance to 0.30 L/min of 100% argon and trace neon and heldfor 5 minutes.

At the completion of the five minute hold, the reactor temperature waslowered to T_(solidus) plus 11° F. while maintaining a temperaturelowering rate of no more than 3° F./hr. Upon reaching T_(solidus) plus11° F., adjust flow rate in the off-centerline lance to 0.30 L/min of100% hydrogen and trace neon. At the completion of flow adjustment, thereactor temperature was lowered to T_(solidus) plus 10° F. whilemaintaining a temperature lowering rate of no more than 3° F./hr. Uponreaching T_(solidus) plus 10° F., adjust flow rate in the off-centerlinelance to 30 ml/min of 100% hydrogen and trace neon. At the completion offlow adjustment, the reactor temperature was lowered to T_(solidus) plus9° F. while maintaining a temperature lowering rate of no more than 3°F./hr. Upon reaching T_(solidus) plus 9° F., the gas addition lance wasrelocated into the headspace of the reactor, such that a quarter inchdimple (e.g., a quarter inch depression) could be observed on the bathsurface. The bath was held at T_(solidus) plus 9° F. for an additional 5minutes for conditioning and equilibration. The reactor was then cooledto T_(solidus) plus 8° F. while maintaining a temperature lowering rateof no more than 3° F./hr. Upon reaching T_(solidus) plus 8° F. a manualpower pulse of 2 kW was introduced with a single continuous up/downsweep from normal holding power. The reactor was then cooled toT_(solidus) plus 2° F. while maintaining a temperature lowering rate ofno more than 3° F./hr. Upon reaching T_(solidus) plus 2° F. a manualpower pulse of 1.5 kW was introduced with a single continuous up/downsweep from normal holding power. Immediately after the 1.5 kW powerpulse, flow was adjusted in the off-centerline lance to 0.15 L/min of50% hydrogen, 50% helium and trace neon. The reactor was then cooled toT_(solidus) again maintaining a temperature-lowering rate of no morethan 3° F./hr. Upon reaching T_(solidus), the induction furnace powersupply was lowered to 1 kW and the reactor was allowed to cool fromT_(solidus) to T_(solidus) minus 75° F. Upon reaching T_(solidus) minus75° F., flow rate in the off-centerline lance was adjusted to 30 ml/minof 60% helium, 40% hydrogen and trace neon. Following the flowadjustment, the induction furnace power supply was lowered to 0.75 kWand the reactor was allowed to cool to 1000° F. Upon reaching 1000° F.,flow rate in the off-centerline lance was adjusted to 30 ml/min of 100%helium and trace neon. Following the flow adjustment, the inductionfurnace power supply was lowered to 0.50 kW and the reactor was allowedto cool to 350° F. Upon reaching 350° F., the induction furnace powersupply was shut down and a timer initiated. At time of 5 minutes, flowrate in the off-centerline lance was adjusted to 0.60 L/min of 100%helium and trace neon. At time of 9 minutes, a neon radiation sourcewithin the sealed enclosure was remotely rotated. Upon completion of therotation, flow in the off-centerline lance was adjusted to 0.30 L/min of88% argon, 12% nitrogen and trace neon.

Following the flow adjustment, the timer was reinitiated. At a time of25 seconds, a neon radiation source within the sealed enclosure wasremotely rotated. At a time of 1 minute 30 seconds, a neon radiationsource within the sealed enclosure was terminated. At a time of 5minutes an argon radiation source within the sealed enclosure wasterminated. At a time of 6 minute 30 seconds, flow rate was adjusted to0.30 L/min of 100% helium and trace neon. At a time of 7 minute, thesecond neon radiation source within the sealed enclosure was terminated.

The timer was reset to zero and restarted. At a time of 15 minutes, thetrace neon gas flow in the off-centerline lance was terminated. At atime of 17 minutes 25 seconds, the xenon radiation source within thesealed enclosure was remotely rotated. At a time of 30 minutes, thetrace helium gas flow in the off-centerline lance was terminated. Thetimer was reset to zero and restarted. At a time of 15 minutes, thexenon radiation source inside the sealed enclosure was terminated.Thirty minutes were allowed to pass. The ingot and crucible were removedfrom the reactor in the presence of radiation sources (metal halidelight sources) utilizing titanium metal tongs.

Upon removal, the crucible was stripped from the metal ingot via agentle wedging action. Immediately following removal, the ingot wastransferred into a quench chamber containing deionized water, ensuringthat the top of the ingot surface was covered by at least 6 inches of DIwater. Upon entrance into the quench chamber, a timer was established.At a time of 2 hours 15 minutes, a long wave ultraviolet radiationsource located above the quench vessel was initiated. At a time of 4hours 7 minutes, a short wave ultraviolet radiation source located abovethe quench vessel was initiated. At a time of 5 hours 59 minutes 30seconds the short wave ultraviolet radiation source located above thequench vessel was rotated to a tip up position.

At a time of 6 hours, the ingot was removed from the quench system usingthe titanium metal tongs and transferred to a clean radiation surfacecountertop. Exposure to external radiation sources included the metalhalide light and placement directly under a skylight (which addedfiltered sunlight to the irradiation sources). The ingot was pat dried.Upon completion of the drying, the long wave ultraviolet radiationsource located above the quench vessel was rotated vertically and movedup 1 inch. The timer was then reset to zero. The ingot was irradiatedfor 10 minutes at which point an additional radiation source (kryptonlamp) was initiated. At 12 minutes 30 seconds, the long wave ultravioletradiation source located above the quench vessel was rotated tohorizontal and moved down to its original position. At 13 minutes, axenon radiation source located above the quench vessel was initiated. At18 minutes, two orthogonal fluorescent lamp racks located next to thecountertop were turned on. At 30 minutes, two angled metal halide lightslocated next to the countertop were simultaneously turned on. At thispoint the timer was again reset. At 13 minutes 15 seconds, a neonradiation source located next to the countertop was turned on. At 15minutes 30 seconds, an argon radiation source located next to thecountertop was turned on. At 23 minutes 45 seconds, the argon radiationsource located next to the countertop was rotated to an angle of 35°. At37 minutes 30 seconds the short wave ultraviolet radiation sourcelocated above the quench vessel was rotated to 350. At 47 minutes 30seconds, the xenon radiation source located above the quench vessel wasrotated to horizontal. At 52 minutes 45 seconds, the long waveultraviolet radiation source located above the quench vessel was rotatedto 350. At 58 minutes 30 seconds, the short wave ultraviolet radiationsource located above the quench vessel was rotated to 55°. At 77minutes, the krypton radiation source located next to the countertop wasrotated to vertical. At 89 minutes, the krypton radiation source locatednext to the countertop was rotated to 78°. At 97 minutes, the kryptonradiation source located next to the countertop was rotated to 88°.

At this point the timer was again reset. At a time of 6 hours, thekrypton lamp, short wave ultraviolet, long wave ultraviolet, argon(located over quench vessel), xenon, argon (located next to countertop),neon, two orthogonal fluorescent lamp racks, and the two angled metalhalide lights were sequentially terminated in the given order. The timerwas again reset. At a time of 6 hours, 30 minutes, normal lab lighting(metal halides) was turned off. The timer was reset. For 48 hours, theingot was allowed to stabilize with no manual intervention (i.e., nohandling).

Example 5 Experimental Procedure for Nickel, Rhenium Method “HD” Run14-01-21

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100-pound induction furnace reactor (Inductotherm)fitted with a 73-30R Powertrak power supply. A gas addition lance wasinstalled to a position approximately ¼ inches from the bottom of thereactor. The reactor was charged with 9080 g nickel (99.9% purity) and 5g rhenium (99.997% purity) through its charging port. The reactor wasfitted with a graphite cap and a ceramic liner (i.e., the crucible, fromEngineering Ceramics). During the entire procedure, a slight positivepressure of 97% argon, 3% hydrogen (˜0.5 psig) was maintained in thereactor using a continuous backspace purge. Bypass injection of gasaddition was commenced (i.e., gas flow diverted around the reactor wasinitiated) at a rate of 0.15 L/min of argon. The incoming gas line forthe gas addition lance passed through a sealed, light-tight enclosurewhereby irradiation of the gas with precise radiation sources (e.g.,wavelength, intensity, etc) was achieved. When the entire gas line hadbeen completely purged (assuming a plug flow model), a neon radiationsource was activated within the sealed enclosure. A timer was initiated.Bypass flow was adjusted to 100% argon at a flow rate of 0.15 L/min withtrace neon present (trace can be defined as ≦0.005% vol. to ≦5%). At atime of 3 minutes, an argon radiation source was activated within thesealed enclosure. After completion of another gas line purge (assuming aplug flow model), the gas line was switched from bypass to directinjection through the gas addition lance.

The induction furnace power was then initiated. The reactor was heatedto 450° F., at a rate no greater than 300° F./hr, as limited by theintegrity of the crucible. The induction furnace operated in thefrequency range of 0 Hz to 3000 Hz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN3000temperature controller. Upon reaching 450° F., the gas addition lancewas repositioned to 2 inches from the bottom of the reactor. The timerwas reinitiated. At a time of 2 minutes, the gas composition was changedto 0.15 L/min of 66% nitrogen, 34% hydrogen and trace neon. Aftercompletion of another gas line purge (assuming a plug flow model), akrypton radiation source was initiated in the sealed enclosure. Thereactor continued to heat up at a rate no greater than 300° F./hr, aslimited by the integrity of the crucible, until T_(solidus) minus 30° F.was achieved. The gas flow rate was then increased to 0.3 L/min with aconstant gas composition. At T_(solidus) a second argon radiation sourcewas activated within the sealed enclosure. Approach T_(solidus) plus 8°F. over a 3 to 5 minute time span. From T_(solidus) plus 8° F. toT_(solidus) plus 15° F., reduce the gas flow rate to 0.15 L/min with aconstant gas composition. Immediately upon reaching T_(solidus) plus 15°F., a second neon radiation source was initiated in the sealedenclosure. Immediately after the second neon radiation source wasinitiated, the gas composition was adjusted to 75% hydrogen, 22%nitrogen, 3% argon, and trace neon. The molten bath was held at thiscondition for 5 minutes for stabilization.

After the 5-minute hold, the gas composition was adjusted to 20% helium,63% nitrogen, 17% argon, and trace neon. The bath was held under theseconditions for an additional 15 minutes. Again, following the hold, thegas composition and flow rate were adjusted to 100% argon with traceneon at a rate of 0.3 L/min. The reactor was held at this condition for3 minutes. The timer was reinitiated. At a time of 65 minutes, graphitesaturation assemblies (⅜ inches OD, 36 inches long high purity (<5 ppmimpurities) graphite rods) were inserted to the bottom of the nickelalloy charge through ports located in the top plate. The nickel washeated to 2540° F. over a one-hour period. The bath was then held atthis condition for 2 hours. Every 30 minutes during the hold period, anattempt was made to lower the graphite saturation assemblies asdissolution occurred. As the nickel became saturated with carbon, thegraphite saturation assemblies were consumed. After the 2-hour holdperiod was complete, the graphite saturation assemblies were removed. Anadditional 40 grams of graphite powder was charged into the reactorthrough the charging port. The bath was then heated to 3390° F. overthree hours. Upon achieving 3390° F., the gas composition and flow ratewere adjusted to 100% nitrogen with trace neon at a rate of 0.3 L/min.The reactor conditions were held for 5 minutes and the gas flow rate wasreduced to 0.15 L/min with constant composition. Immediately followingthis reduction in gas flow, the krypton radiation source in the sealedenclosure was turned off. The timer was reinitiated. At a time of 3minutes, the gas flow rate was reduced to 37.5 ml/min with constantcomposition. One of the argon radiation sources inside the sealedenclosure was turned off. At a time of 5 minutes, the nitrogen componentof the gas flow was discontinued, while maintaining the flow of thetrace neon. At a time of 10 minutes, one of the neon radiation sourceswithin the sealed enclosure was remotely rotated. The reactortemperature was lowered to 3193° F. over 7 minutes.

The temperature was then varied between 2897° F. and 3193° F. for 16cycles. Each cycle consisted of raising the temperature continuouslyover 7 minutes and lowering the temperature continuously over 7 minutes.After completion of the 14.5 cycles, argon is reintroduced at a flowrate of 0.15 L/min with trace neon. Five minutes into the 15^(th) cycle,a xenon radiation source was activated within the sealed enclosure. At 6minutes into the 15^(th) cycle, a long wave ultraviolet radiation sourcewas activated in the sealed enclosure. At sweep count 15.5, a short waveultraviolet radiation source was initiated in the sealed enclosure. Atsweep count 16, remotely rotate the xenon radiation source within thesealed enclosure. The temperature of the nickel was varied over another5 cycles between 2897° F. and 3193° F. After the fifth cycle, thereactor temperature was lowered to 2800° F. over a 60-minute period.Upon achieving the target temperature of 2800° F., the graphitesaturation assemblies were reinstalled in the nickel and remained therefor 1 hour. The graphite saturation assemblies were then removed.

Two voltage probes (source and ground probe) were then installed in theheadspace of the reactor and allowed to equilibrate for 5 minutes. Uponcompletion of the five-minute hold, the voltage probes are lowered intothe bath. The source probe was positioned 2 inches below the axialcenter and 1 inch from the radial center. The ground probe waspositioned 0.75 inches above the axial position of the source probe and1 inch from the radial center (180° from the source probe). Once theprobes were installed, a five-minute hold at this condition was done toallow the bath to electronically equilibrate with the probes. Voltagewas then applied to the probes and varied between multiple voltage setpoints. This voltage was in a continuous up/down sweep between twopredetermined voltages. The first voltage cycle was varied between 17and 18 volts for 24 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The second voltage cycle was varied between 13.25 and 14.75volts for 20 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The third voltage cycle was varied between 8.75 and 10.25volts for 17 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The fourth voltage cycle was varied between 4.00 and 7.00volts for 14 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The fifth voltage cycle was varied between 1.50 and 5.00volts for 10 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The sixth voltage cycle was varied between 0.50 and 2.00volts for 3 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. When the final cycle was completed the voltage was set ontoa constant 1-volt setting. This voltage remained constant until a laterstep during which the leads were removed.

The reactor temperature was then lowered to 2780° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued gasaddition. The temperature was then varied between 2741° F. and 2780° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. After the 20^(th) cycle, turning off the argon componentof the gas leaving only traces of neon gas flow changed third body gasaddition. The bath was then cooled to 2722° F. over 5 minutes. Uponreaching 2722° F., one of the neon radiation sources within the sealedenclosure was remotely rotated.

The temperature was then varied between 2664° F. and 2722° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 0.15 L/min flow of 60%argon, 40% helium, and trace neon was added, and while lowering thetemperature, a 0.3 L/min flow of 100% helium, trace neon, and tracekrypton was added. At sweep count 0.5, a krypton radiation source wasinitiated in the sealed enclosure. At sweep count 1.0, an argonradiation source was initiated in the sealed enclosure. At sweep count4.5, a short wave ultraviolet radiation source was terminated in thesealed enclosure. The reactor temperature was lowered to 2645° F. over 5minutes. The temperature was varied between 2451° F. and 2645° F. for15.5 cycles. Each cycle consisted of lowering the temperaturecontinuously over 15 minutes and raising the temperature continuouslyover 15 minutes. In addition, while raising the temperature, a 0.15L/min flow of 60% argon, 40% helium, and trace neon was added, and whilelowering the temperature, a 0.3 L/min flow of 100% helium, trace neon,and trace krypton was added. After the 15.5^(th) cycle, turning off allgas components except the trace neon gas flow changed third body gasaddition.

After the 15.5^(th) cycle, a timer was initiated. At a time of 3minutes, the xenon radiation source within the sealed enclosure wasremotely rotated. The timer was reinitiated. At 60 minutes, flow rateswere adjusted to 0.3 L/min of 100% argon and trace neon. At 65 minutes,flow rates were adjusted to 3.0 ml/min of 60% argon, 40% helium, andtrace neon. Immediately after the flow was adjusted, remotely rotate oneof the neon radiation sources within the sealed enclosure. At 68minutes, flow rates were adjusted to 0.15 L/min of 100% helium, traceneon and trace krypton. At 68 minutes 20 seconds, the 1-volt power wasbrought to zero output and the voltage power leads removed from thevoltage probes. At 68 minutes 30 seconds, the long wave ultravioletradiation source was turned off in the sealed enclosure. At 71 minutes15 seconds, reposition the voltage probes to three inches above the bathsurface. At 75 minutes, remove the source and ground probes completelyfrom the reactor.

After the voltage probes had been removed from the reactor, flow rateswere adjusted to 0.15 L/min of 77% argon, 18% nitrogen, 5% helium, andtrace neon. The reactor was then held at temperature and flow rate for15 minutes. After the 15-minute hold, an argon radiation source wasturned off in the sealed enclosure. The flow rates were immediatelyreadjusted to the flow rate 0.15 L/min of 77% argon, 12% nitrogen, 11%helium, and trace neon. The reactor was then held at temperature andflow rate for 25 minutes. After the 25-minute hold, the kryptonradiation source was turned off in the sealed enclosure. The flow rateswere immediately readjusted to the flow rate 0.30 L/min of 10% argon,90% helium and trace neon. The reactor was then held at temperature andflow rate for 3 minutes. After the 3-minute hold, flow rates wereadjusted to 0.15 L/min of 10% argon, 90% helium and trace neon and heldfor 2 minutes. After the 2-minute hold, flow rates were adjusted to 0.30L/min of 7% hydrogen, 93% nitrogen and trace neon and held for 10minutes. After the 10-minute hold, flow rates were adjusted to the flowrate of 0.15 L/min of 7% hydrogen, 93% nitrogen and trace neon and heldfor 3 minutes. After the 3-minute hold, flow rates were adjusted to 30ml/min of 7% hydrogen, 93% nitrogen and trace neon and held for 2minutes. After the 2-minute hold, flow rates were adjusted to 0.15 L/minof 87% argon, 10% nitrogen, 3% helium, and trace neon and held for 5minutes. After the 5-minute hold, flow rates were adjusted to 0.6 L/minof 90% argon, 10% nitrogen and trace neon and held for 7 minutes. Afterthe 7-minute hold, flow rates were adjusted to 30 ml/min of 90% argon,10% nitrogen and trace neon and held for 2 minutes. After the 2-minutehold, flow rates were adjusted to 0.60 L/min of 95% argon, 5% nitrogenand trace neon and held for 15 minutes. After the 15-minute hold, flowrates were adjusted to 0.30 L/min of 95% argon, 5% nitrogen and traceneon and held for 5 minutes.

The reactor temperature was lowered to 2529° F. over 21 minutes. Thetemperature was then varied between 2451° F. and 2529° F. for threecycles. The cycle consisted of raising the temperature continuously over27 minutes and lowering the temperature continuously over 27 minutes.After the third cycle, the bath was held at 2529° F. for 5 minutes. Thereactor temperature was then lowered to 2451° F. over 2 minutes 30seconds. The temperature was then varied between 2529° F. and 2451° F.for two cycles. The cycles consisted of raising the temperaturecontinuously over 11 minutes and lowering the temperature continuouslyover 7 minutes.

After completion of the 2^(nd) cycle, the induction power supply wasplaced into manual control. The power was then instantaneously increased5 kW above the steady state power level and immediately upon hitting the5 kW increase the power was instantaneously decreased back to the steadystate power level. The power level was then varied up 3.7 kW and down3.7 kW over 6 cycles. The cycles consisted of raising power 3.7 kW abovethe steady state power level over 25 seconds. Once raised, the powerlevel was held at the additional 3.7 kW setting for 45 seconds.Following the 45 second hold, the power was lowered back to the steadystate power level over a 15 second time frame.

After the 6^(th) power cycle, the gas flows were adjusted to 0.60 L/minof 100% argon and trace neon and held for 7 minutes. Following theseven-minute hold, the argon flow was secured leaving only the traceneon flow. Once the argon flow was secured, a second lance waspositioned inside the reactor. This lance was placed at a distance ⅔from the radial center and 1.5 inches from the bottom of the bath. Thecenterline lance was then repositioned to ¼ inch from the bottom. Oncethe centerline lance was repositioned, flow was started in theoff-centerline lance at a rate of 30 ml/min of 100% argon and traceneon. A timer was reinitiated. At a time of 2 minutes, the trace neonflow in the centerline lance was secured. At a time of 2 minutes 30seconds, flow was initiated in the centerline lance at a flow rate of 30ml/min of 100% carbon monoxide and held for 3 minutes. After the3-minute hold, flow rates were adjusted in the off-centerline lance to0.15 L/min of 100% argon and trace neon and held for 15 minutes. Afterthe 15-minute hold, flow rates were adjusted in the off-centerline lanceto trace neon only. Furthermore, the flow rate was adjusted in thecenterline lance to 0.60 L/min of 100% carbon monoxide and held for 10minutes. After the 10-minute hold, the carbon monoxide in the centerlinelance was secured. The reactor temperature was then lowered toT_(solidus) plus 18° F. over 30 minutes. Upon reaching the T_(solidus)plus 18° F., flow was adjusted in the centerline lance to 0.30 L/min of100% carbon monoxide and held for 20 minutes. After the 20-minute hold,all flow was secured in the centerline lance and the lance was removed.

After the centerline lance was removed, flow rates in the off-centerlinelance were adjusted to 30 ml/min of 88% argon, 12% nitrogen and traceneon, and held for 3 minutes. After the 3-minute hold, flow rates wereadjusted to 0.30 L/min of 25% helium, 75% argon and trace neon and heldfor 10 minutes. After the 10-minute hold, flow rates were adjusted to0.30 L/min of 88% argon, 12% nitrogen and trace neon and held for 10minutes. After the 10-minute hold, flow rates were adjusted to 0.15L/min of 88% argon, 12% nitrogen and trace neon and held for 5 minutes.After the 5-minute hold, flow rates were adjusted to 30 m/min of 88%argon, 12% nitrogen and trace neon and held for 2 minutes. After the2-minute hold, flow rates were adjusted to 0.15 L/min of 88% argon, 12%nitrogen and trace neon. Once the flow rate was adjusted, the reactortemperature was lowered to T_(solidus) plus 15° F. over 45 minutes. Uponreaching the T_(solidus) plus 15° F., flow was adjusted in theoff-centerline lance to 0.30 L/min of 100% argon and trace neon and heldfor 5 minutes.

At the completion of the five minute hold, the reactor temperature waslowered to T_(solidus) plus 11° F. while maintaining a temperaturelowering rate of no more than 3° F./hr. Upon reaching T_(solidus) plus11° F., flow rate in the off-centerline lance was adjusted to 0.30 L/minof 100% hydrogen and trace neon. At the completion of flow adjustment,the reactor temperature was lowered to T_(solidus) plus 10° F. whilemaintaining a temperature lowering rate of no more than 3° F./hr. Uponreaching T_(solidus) plus 10° F., flow rate in the off-centerline lancewas adjusted to 30 ml/min of 100% hydrogen and trace neon. At thecompletion of the flow adjustment, the reactor temperature was loweredto T_(solidus) plus 9° F. while maintaining a temperature-lowering rateof no more than 3° F./hr. Upon reaching T_(solidus) plus 9° F., the gasaddition lance was relocated into the headspace of the reactor, suchthat a quarter inch (¼ inches) dimple could be observed on the bathsurface. The bath was held at T_(solidus) plus 9° F. for an additional 5minutes for conditioning and equilibration. The reactor was then cooledto T_(solidus) plus 8° F. while maintaining a temperature lowering rateof no more than 3° F./hr. Upon reaching T_(solidus) plus 8° F. a manualpower pulse of 2 kW was introduced with a single continuous up/downsweep from normal holding power. The reactor was then cooled toT_(solidus) plus 2° F. while maintaining a temperature lowering rate ofno more than 3° F./hr. Upon reaching T_(solidus) plus 2° F. a manualpower pulse of 1.5 kW was introduced with a single continuous up/downsweep from normal holding power. Immediately after the 1.5 kW powerpulse, flow was adjusted in the off-centerline lance to 0.15 L/min of50% hydrogen, 50% helium and trace neon. The reactor was then cooled toT_(solidus) again maintaining a temperature-lowering rate of no morethan 3° F./hr. Upon reaching T_(solidus), the induction furnace powersupply was lowered to 1 kW and the reactor was allowed to cool fromT_(solidus) to T_(solidus) minus 75° F. Upon reaching T_(solidus) minus75° F., adjust flow rate in the off-centerline lance to 30 m/min of 60%helium, 40% hydrogen and trace neon. Following the flow adjustment, theinduction furnace power supply was lowered to 0.75 kW and the reactorwas allowed to cool to 1000° F. Upon reaching 1000° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 100% helium and traceneon. Following the flow adjustment, the induction furnace power supplywas lowered to 0.50 kW and the reactor was allowed to cool to 350° F.Upon reaching 350° F., the induction furnace power supply was shut downand a timer initiated. At a time of 5 minutes, flow rate in theoff-centerline lance was adjusted to 0.60 L/min of 100% helium and traceneon. At a time of 9 minutes, a neon radiation source within the sealedenclosure was remotely rotated. Upon completion of the rotation, flow inthe off-centerline lance was adjusted to 0.30 L/min of 88% argon, 12%nitrogen and trace neon.

Following the flow adjustment, the timer was reinitiated. At a time of25 seconds, a neon radiation source within the sealed enclosure wasremotely rotated. At a time of 1 minute 30 seconds, a neon radiationsource within the sealed enclosure was terminated. At a time of 5minutes, an argon radiation source within the sealed enclosure wasterminated. At a time of 6 minutes 30 seconds, flow rate was adjusted to0.30 L/min of 100% helium and trace neon. At a time of 7 minute, thesecond neon radiation source within the sealed enclosure was terminated.

The timer was reinitiated. At a time of 15 minutes, the trace neon gasflow in the off-centerline lance was terminated. At a time of 17 minutes25 seconds, the xenon radiation source within the sealed enclosure wasremotely rotated. At a time of 30 minutes, the trace helium gas flow inthe off-centerline lance was terminated. The timer was reinitiated. At atime of 15 minutes, the xenon radiation source inside the sealedenclosure was terminated. Thirty minutes were allowed to pass. The ingotand crucible were removed from the reactor in the presence of radiationsources (metal halide light sources) utilizing titanium metal tongs.

Upon removal, the crucible was stripped from the metal ingot via agentle wedging action. Immediately following removal, the ingot wastransferred into a quench chamber containing deionized water, ensuringthat the top of the ingot surface was covered by at least 6 inches of DIwater. Upon entrance into the quench chamber, a timer was established.At a time of 2 hours 15 minutes, a long wave ultraviolet radiationsource located above the quench vessel was initiated. At a time of 4hours 7 minutes, a short wave ultraviolet radiation source located abovethe quench vessel was initiated. At a time of 5 hours 59 minutes 30seconds, the short wave ultraviolet radiation source located above thequench vessel was rotated to a vertical position.

At a time of 6 hours, the ingot was removed from the quench system usingthe titanium metal tongs and transferred to a clean radiation surfacecountertop. Exposure to external radiation sources included the metalhalide light and placement directly under a skylight (which addedfiltered sunlight to the irradiation sources). The ingot was pat dried.Upon completion of the drying, the long wave ultraviolet radiationsource located above the quench vessel was rotated vertical and moved up1 inch. The timer was then reinitiated. The ingot was irradiated for 10minutes at which point an additional radiation source (krypton lamp) wasinitiated. At 12 minutes 30 seconds, the long wave ultraviolet radiationsource located above the quench vessel was rotated horizontal and moveddown to its original position. At 13 minutes, a xenon radiation sourcelocated above the quench vessel was initiated. At 18 minutes, twoorthogonal fluorescent lamp racks located next to the countertop wereturned on. At 30 minutes, two angled metal halide lights located next tothe countertop were simultaneously turned on. At this point the timerwas again reinitiated. At 13 minutes 15 seconds, a neon radiation sourcelocated next to the countertop was turned on. At 15 minutes 30 seconds,an argon radiation source located next to the countertop was turned on.At 23 minutes 45 seconds, the argon radiation source located next to thecountertop was rotated to an angle of 350. At 37 minutes 30 seconds, theshort wave ultraviolet radiation source located above the quench vesselwas rotated to 35°. At 47 minutes 30 seconds, the xenon radiation sourcelocated above the quench vessel was rotated to horizontal. At 52 minutes45 seconds, the long wave ultraviolet radiation source located above thequench vessel was rotated to 35°. At 58 minutes 30 seconds, the shortwave ultraviolet radiation source located above the quench vessel wasrotated to 55°. At 77 minutes, the krypton radiation source located nextto the countertop was rotated to vertical. At 89 minutes, the kryptonradiation source located next to the countertop was rotated 78°. At 93minutes, the ingot was lifted using composite black rubber gloves and atailored material that acts as an energy filter was placed under theingot. The tailored material used as an energy filter has an XRF asdepicted in the Appendix 1. The ingot was then lowered onto the tailoredenergy filter.

At this point the timer was again reset. At a time of 6 hours, thekrypton lamp, short wave ultraviolet, long wave ultraviolet, argon(located over quench vessel), xenon, argon (located next to countertop),neon, two orthogonal fluorescent lamp racks, and the two angled metalhalide lights were sequentially terminated in the given order. The timerwas again reset. At a time of 6 hours, 30 minutes, normal lab lighting(metal halides) was turned off. The timer was reset. For 48 hours, theingot was allowed to stabilize with no manual intervention (i.e., nohandling).

Example 6 Experimental Procedure for Iron, Vanadium, Chromium, ManganeseMethod “HD” Run 14-01-13

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100-pound induction furnace reactor (Inductotherm)fitted with a 73-30R Powertrak power supply. A gas addition lance wasinstalled to a position approximately ¼ inches from the bottom of thereactor. The reactor was charged with 8534 g iron (99.98% purity), 182 gvanadium (99.5% purity), 182 g chromium (99.999% purity) and 182 gmanganese (99.99% purity) through its charging port. The reactor wasfitted with a graphite cap and a ceramic liner (i.e., the crucible, fromEngineering Ceramics). During the entire procedure, a slight positivepressure of 97% argon, 3% hydrogen (˜0.5 psig) was maintained in thereactor using a continuous backspace purge. Bypass injection of gasaddition was commenced (i.e., gas flow diverted around the reactor wasinitiated) at a rate of 0.15 L/min of argon. The incoming gas line forthe gas addition lance passed through a sealed, light-tight enclosurewhereby irradiation of the gas with precise radiation sources (e.g.,wavelength, intensity, etc) was achieved. When the entire gas line hadbeen completely purged (assuming a plug flow model), a neon radiationsource was activated within the sealed enclosure. A timer was initiated.Bypass flow was adjusted to 100% argon at a flow rate of 0.15 L/min withtrace neon present (trace can be defined as ≦0.005% volume to ≦5%). At atime of 3 minutes, an argon radiation source was activated within thesealed enclosure. After completion of another gas line purge (assuming aplug flow model), the gas line was switched from bypass to directinjection through the gas addition lance.

The induction furnace power was then initiated. The reactor was heatedto 450° F., at a rate no greater than 300° F./hr, as limited by theintegrity of the crucible. The induction furnace operated in thefrequency range of 0 Hz to 3000 Hz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN3000temperature controller. Upon reaching 450° F., the gas addition lancewas repositioned to 2 inches from the bottom of the reactor. The timerwas reinitiated. At a time of 2 minutes, the gas composition was changedto 0.15 L/min of 66% nitrogen, 34% hydrogen and trace neon. Aftercompletion of another gas line purge (assuming a plug flow model), akrypton radiation source was initiated in the sealed enclosure. Thereactor heat up continued at a rate no greater than 300° F./hr, aslimited by the integrity of the crucible, until T_(solidus) minus 30° F.was achieved. The gas flow rate was then increased to 0.3 L/min with aconstant gas composition. At T_(solidus) a second argon radiation sourcewas activated within the sealed enclosure. Approach T_(solidus) plus 8°F. over a 3 to 5 minute time span. From T_(solidus) plus 8° F. toT_(solidus) plus 15° F., reduce the gas flow rate to 0.15 L/min with aconstant gas composition. Immediately upon reaching T_(solidus) plus 15°F., a second neon radiation source was initiated in the sealedenclosure. Immediately after the second neon radiation source wasinitiated, the gas composition was adjusted to 75% hydrogen, 22%nitrogen, 3% argon, and trace neon. The molten bath was held at thiscondition for 5 minute for stabilization.

After the 5-minute hold, the gas composition was adjusted to 20% helium,63% nitrogen, 17% argon, and trace neon. The bath was held under theseconditions for an additional 15 minutes. Again, following the hold, thegas composition and flow rate were adjusted to 100% argon with traceneon at a rate of 0.3 L/min. The reactor was held at this condition for3 minutes. The timer was reinitiated. At a time of 65 minutes, graphitesaturation assemblies (⅜ inches OD, 36 inches long high purity (<5 ppmimpurities) graphite rods) were inserted to the bottom of the iron alloycharge through ports located in the top plate. The iron was cooled to2243° F. over a two-hour period. The bath was cooled due to thet-solidus temperature of an iron bath with no carbon versus thetemperature requirement of a carbon-containing bath. The bath was thenheld at this condition for 2 hours. Every 30 minutes during the holdperiod, an attempt was made to lower the graphite saturation assembliesas dissolution occurred. As the iron alloy became saturated with carbon,the graphite saturation assemblies were consumed. After the 2-hour holdperiod was complete, the graphite saturation assemblies were removed. Anadditional 90 grams of graphite powder was charged into the reactorthrough the charging port. The bath was then heated to 3525° F. overthree hours. Upon achieving 3525° F., the gas composition and flow ratewere adjusted to 100% nitrogen with trace neon at a rate of 0.3 L/minand held for 5 minutes. Reduce the gas flow rate to 0.15 L/min withconstant composition. Immediately following this reduction in gas flow,the krypton radiation source in the sealed enclosure was turned off. Thetimer was reinitiated. At a time of 3 minutes, the gas flow rate wasreduced to 37.5 ml/min with constant composition. One of the argonradiation sources inside the sealed enclosure was turned off. At a timeof 5 minutes, the nitrogen component of the gas flow was discontinuedwhile maintaining the flow of the trace neon. At a time of 10 minutes,one of the neon radiation sources within the sealed enclosure wasremotely rotated. The reactor temperature was lowered to 3360° F. over 7minutes.

The temperature was then varied between 2993° F. and 3360° F. for 16cycles. Each cycle consisted of raising the temperature continuouslyover 7 minutes and lowering the temperature continuously over 7 minutes.After completion of the 14.5 cycles, argon was reintroduced at a flowrate of 0.15 L/min with trace neon. Five minutes into the 15^(th) cycle,a xenon radiation source was activated within the sealed enclosure. At 6minutes into the 15^(th) cycle, a long wave ultraviolet radiation sourcewas activated in the sealed enclosure. At sweep count 15.5, a short waveultraviolet radiation source was initiated in the sealed enclosure. Atsweep count 16, the xenon radiation source within the sealed enclosurewas remotely rotated. The temperature of the iron alloy was varied overanother 5 cycles between 2993° F. and 3360° F. After the fifth cycle,the reactor temperature was then lowered to 2850° F. over a 60-minuteperiod. Upon achieving the target temperature of 2850, the graphitesaturation assemblies were reinstalled in the iron alloy and remainedthere for 1 hour. The graphite saturation assemblies were then removed.

Two voltage probes (source and ground probe) were then installed in theheadspace of the reactor and allowed to equilibrate for 5 minutes. Uponcompletion of the five-minute hold the voltage probes were lowered intothe bath. The source probe was positioned 2 inches below the axialcenter and 1 inch from the radial center. The ground probe waspositioned 0.75 inches above the axial position of the source probe and1 inch from the radial center (180° from the source probe). Once theprobes were installed a five-minute hold at this condition was done toallow the bath to electronically equilibrate with the probes. Voltagewas then applied to the probes and varied between multiple voltage setpoints. This voltage was in a continuous up/down sweep between twopredetermined voltages. The first voltage cycle was varied between 17and 18 volts for 24 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The second voltage cycle was varied between 13.25 and 14.75volts for 20 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The third voltage cycle was varied between 8.75 and 10.25volts for 17 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The fourth voltage cycle was varied between 4.00 and 7.00volts for 14 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The fifth voltage cycle was varied between 1.50 and 5.00volts for 10 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. The sixth voltage cycle was varied between 0.50 and 2.00volts for 3 cycles. Each cycle consisted of raising the voltagecontinuously over 45 seconds and lowering the voltage continuously over45 seconds. When the final cycle was completed the voltage was set ontoa constant 1-volt setting. This voltage remains constant until a laterstep when the leads are removed.

The reactor temperature was lowered to 2819° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued gasaddition. The temperature was then varied between 2757° F. and 2819° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. After the 20^(th) cycle, turning off the argon componentof the gas leaving only trace neon gas flow changed third body gasaddition. The bath was then cooled to 2724° F. over 5 minutes. Uponreaching 2724° F., one of the neon radiation sources within the sealedenclosure was remotely rotated.

The temperature was then varied between 2622° F. and 2724° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 0.15 L/min flow of 60%argon, 40% helium, and trace neon was added, and while lowering thetemperature, a 0.3 L/min flow of 100% helium, trace neon, and tracekrypton was added. At sweep count 0.5, a krypton radiation source wasinitiated in the sealed enclosure. At sweep count 1.0, an argonradiation source was initiated in the sealed enclosure. At sweep count4.5, a short wave ultraviolet radiation source was terminated in thesealed enclosure. The reactor temperature was lowered to 2586° F. over 5minutes. The temperature was varied between 2133° F. and 2586° F. for15.5 cycles. Each cycle consisted of lowering the temperaturecontinuously over 15 minutes and raising the temperature continuouslyover 15 minutes. In addition, while raising the temperature, a 0.15L/min flow of 60% argon, 40% helium, and trace neon was added, and whilelowering the temperature, a 0.3 L/min flow of 100% helium, trace neon,and trace krypton was added. After the 15.5^(th) cycle, turning off allgas components except the trace neon gas flow changed third body gasaddition.

After the 15.5^(th) cycle, a timer was initiated. At a time of 3minutes, remotely rotate the xenon radiation source within the sealedenclosure. The timer was then reinitiated. At 60 minutes, flow rateswere adjusted to 0.3 L/min of 100% argon and trace neon. At 65 minutes,flow rates were adjusted to 30 ml/min of 60% argon, 40% helium, andtrace neon. Immediately after the flow was adjusted, one of the neonradiation sources within the sealed enclosure was remotely rotated. At68 minutes, flow rates were adjusted to 0.15 L/min of 100% helium, traceneon and trace krypton. At 68 minutes 20 seconds, the 1-volt power wasbrought to zero output and the voltage power leads removed from thevoltage probes. At 68 minutes 30 seconds, the long wave ultravioletradiation source was turned off in the sealed enclosure. At 71 minutes15 seconds, the voltage probes were repositioned to three inches abovethe bath surface. At 75 minutes, the source and ground probe wereremoved completely from the reactor.

After the voltage probes had been removed from the reactor, flow rateswere adjusted to 0.15 L/min of 77% argon, 18% nitrogen, 5% helium, andtrace neon. The reactor was then held at temperature and flow rate for15 minutes. After the 15-minute hold, an argon radiation source wasturned off in the sealed enclosure. The flow rates were immediatelyreadjusted to the flow rate 0.15 L/min of 77% argon, 12% nitrogen, 11%helium, and trace neon. The reactor was then held at temperature andflow rate for 25 minutes. After the 25-minute hold, the kryptonradiation source was turned off in the sealed enclosure. The flow rateswere immediately readjusted to a flow rate of 0.30 L/min of 10% argon,90% helium and trace neon. The reactor was then held at temperature andflow rate for 3 minutes. After the 3-minute hold, flow rates wereadjusted to 0.15 L/min of 10% argon, 90% helium and trace neon and heldfor 2 minutes. After the 2-minute hold, flow rates were adjusted to 0.30L/min of 7% hydrogen, 93% nitrogen and trace neon and held for 10minutes. After the 10-minute hold, flow rates were adjusted to 0.15L/min of 7% hydrogen, 93% nitrogen and trace neon and held for 3minutes. After the 3-minute hold, flow rates were adjusted to 30 ml/minof 7% hydrogen, 93% nitrogen and trace neon and held for 2 minutes.After the 2-minute hold, flow rates were adjusted to 0.15 L/min of 87%argon, 10% nitrogen, 3% helium, and trace neon and held for 5 minutes.After the 5-minute hold, flow rates were adjusted to 0.6 L/min of 90%argon, 10% nitrogen and trace neon and held for 7 minutes. After the7-minute hold, flow rates were adjusted to 30 ml/min of 90% argon, 10%nitrogen and trace neon and held for 2 minutes. After the 2-minute hold,flow rates were adjusted to 0.60 L/min of 95% argon, 5% nitrogen andtrace neon and held for 15 minutes. After the 15-minute hold, flow rateswere adjusted to 0.30 L/min of 95% argon, 5% nitrogen and trace neon andheld for 5 minutes.

The reactor temperature was raised to 2340° F. over 21 minutes. Thetemperature was then varied between 2133° F. and 2340° F. for threecycles. The cycle consisted of raising the temperature continuously over27 minutes and lowering the temperature continuously over 27 minutes.After the third cycle, the bath was held at 2340° F. for 5 minutes. Thereactor temperature was then lowered to 2133° F. over 2 minutes 30seconds. The temperature was then varied between 2340° F. and 2133° F.for two cycles. The cycle consisted of raising the temperaturecontinuously over 11 minutes and lowering the temperature continuouslyover 7 minutes.

After completion of the 2^(nd) cycle, the induction power supply wasplaced into manual control. The power was then instantaneously increased5 kW above the steady state power level and immediately upon hitting the5 kW increased the power was instantaneously decreased back to thesteady state power level. The power level was then varied up 3.7 kW anddown 3.7 kW over 6 cycles. The cycles consisted of raising power 3.7 kWabove the steady state power level over 25 seconds. Once raised, thepower level was held at the additional 3.7 kW setting for 45 seconds.Following the 45 second hold, the power was lowered back to the steadystate power level over a 15 second time frame.

After completion of the 6^(th) power cycle, the gas flows were adjustedto 0.60 L/min of 100% argon and trace neon and held for 7 minutes.Following the seven-minute hold, the argon flow was secured leaving onlythe trace neon flow. Once the argon flow was secured, a second lance waspositioned inside the reactor. This lance was placed at a distance ⅔from the radial center and 1.5 inches from the bottom of the bath. Thecenterline lance was then repositioned to ¼ inch from the bottom. Oncethe centerline lance was repositioned, flow was started in theoff-centerline lance at a rate of 30 ml/min of 100% argon and traceneon. A timer was initiated. At a time of 2 minutes, the trace neon flowin the centerline lance was secured. At a time of 2 minutes 30 seconds,flow was initiated in the centerline lance at a flow rate of 30 ml/minof 100% carbon monoxide and held for 3 minutes. After the 3-minute hold,flow rates were adjusted in the off-centerline lance to 0.15 L/min of100% argon and trace neon and held for 15 minutes. After the 15-minutehold, flow rates were adjusted in the off-centerline lance to trace neononly. Furthermore, the flow rate was adjusted in the centerline lance to0.60 L/min of 100% carbon monoxide and held for 10 minutes. After the10-minute hold, the carbon monoxide in the centerline lance was secured.The reactor temperature was then lowered to T_(solidus) plus 18° F. over30 minutes. Upon reaching the T_(solidus) plus 18° F., flow was adjustedin the centerline lance to 0.30 L/min of 100% carbon monoxide and heldfor 20 minutes. After the 20-minute hold, all flow was secured in thecenterline lance and the lance was removed.

After the centerline lance was removed, adjust flow rates in theoff-centerline lance to 30 ml/min of 88% argon, 12% nitrogen and traceneon and held for 3 minutes. After the 3-minute hold, flow rates wereadjusted to 0.30 L/min of 25% helium, 75% argon and trace neon and heldfor 10 minutes. After the 10-minute hold, flow rates were adjusted to0.30 L/min of 88% argon, 12% nitrogen and trace neon and held for 10minutes. After the 10-minute hold, flow rates were adjusted to 0.15L/min of 88% argon, 12% nitrogen and trace neon and held for 5 minutes.After the 5-minute hold, flow rates were adjusted to 30 cc/min of 88%argon, 12% nitrogen and trace neon and held for 2 minutes. After the2-minute hold, flow rates were adjusted to 0.15 L/min of 88% argon, 12%nitrogen and trace neon. Once the flow rate was adjusted, the reactortemperature was lowered to T_(solidus) plus 15° F. over 45 minutes. Uponreaching the T_(solidus) plus 15° F., flow was adjusted in theoff-centerline lance to 0.30 L/min of 100% argon and trace neon and heldfor 5 minutes.

At the completion of five minute hold, the reactor temperature waslowered to T_(solidus) plus 11° F. while maintaining a temperaturelowering rate of no more than 3° F./hr. Upon reaching T_(solidus) plus11° F., flow rate in the off-centerline lance was adjusted to 0.30 L/minof 100% hydrogen and trace neon. At the completion of the flowadjustment, the reactor temperature was then lowered to T_(solidus) plus10° F. while maintaining a temperature lowering rate of no more than 3°F./hr. Upon reaching T_(solidus) plus 10° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 100% hydrogen andtrace neon. At the completion of the flow adjustment, the reactortemperature was lowered to T_(solidus) plus 9° F. while maintaining atemperature-lowering rate of no more than 3° F./hr. Upon reachingT_(solidus) plus 9° F., the gas addition lance was relocated into theheadspace of the reactor, such that a quarter inch (¼ inches) dimplecould be observed on the bath surface. The bath was held at T_(solidus)plus 9° F. for an additional 5 minutes for conditioning andequilibration. The reactor was then cooled to T_(solidus) plus 8° F.while maintaining a temperature lowering rate of no more than 3° F./hr.Upon reaching T_(solidus) plus 8° F. a manual power pulse of 2 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. The reactor was then cooled to T_(solidus) plus 2° F. whilemaintaining a temperature lowering rate of no more than 3° F./hr. Uponreaching T_(solidus) plus 2° F. a manual power pulse of 1.5 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. Immediately after the 1.5 kW power pulse, flow was adjusted inthe off-centerline lance to 0.15 L/min of 50% hydrogen, 50% helium andtrace neon. The reactor was then cooled to T_(solidus) again maintaininga temperature-lowering rate of no more than 3° F./hr. Upon reachingT_(solidus), the induction furnace power supply was lowered to 1 kW andthe reactor was allowed to cool from T_(solidus) to T_(solidus) minus75° F. Upon reaching T_(solidus) minus 75° F., flow rate in theoff-centerline lance was adjusted to 30 m/min of 60% helium, 40%hydrogen and trace neon. Following the flow adjustment, the inductionfurnace power supply was lowered to 0.75 kW and the reactor was allowedto cool to 1000° F. Upon reaching 1000° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 100% helium and traceneon. Following the flow adjustment, the induction furnace power supplywas lowered to 0.50 kW and the reactor was allowed to cool to 350° F.Upon reaching 350° F., the induction furnace power supply was shut downand the timer reinitiated. At a time of 5 minutes, flow rate in theoff-centerline lance was adjusted to 0.60 L/min of 100% helium and traceneon. At a time of 9 minutes, a neon radiation source within the sealedenclosure was remotely rotated. Upon completion of the rotation, flow inthe off-centerline lance was adjusted to 0.30 L/min of 88% argon, 12%nitrogen and trace neon.

Following the flow adjustment, the timer was reinitiated. At a time of25 seconds, a neon radiation source within the sealed enclosure wasremotely rotated. At a time of 1 minute 30 seconds, a neon radiationsource within the sealed enclosure was terminated. At a time of 5minutes an argon radiation source within the sealed enclosure wasterminated. At a time of 6 minute 30 seconds, flow rate was adjusted to0.30 L/min of 100% helium and trace neon. At a time of 7 minute, thesecond neon radiation source within the sealed enclosure was terminated.

The timer was reinitiated. At a time of 15 minutes, the trace neon gasflow in the off-centerline lance was terminated. At a time of 17 minutes25 seconds, the xenon radiation source within the sealed enclosure wasremotely rotated. At a time of 30 minutes, the trace helium gas flow inthe off-centerline lance was terminated. The timer was reinitiated. At atime of 15 minutes, the xenon radiation source inside the sealedenclosure was terminated. Thirty minutes were allowed to pass. The ingotand crucible were removed from the reactor in the presence of radiationsources (metal halide light sources) utilizing titanium metal tongs.

Upon removal, the crucible was stripped from the metal ingot via agentle wedging action. Immediately following removal, the ingot wastransferred into a quench chamber containing deionized water, ensuringthat the top of the ingot surface was covered by at least 6 inches of DIwater. Upon entrance into the quench chamber, a timer was initiated. Ata time of 2 hours 15 minutes, a long wave ultraviolet radiation sourcelocated above the quench vessel was initiated. At a time of 4 hours 7minutes, a short wave ultraviolet radiation source located above thequench vessel was initiated. At a time of 5 hours 59 minutes 30 seconds,the short wave ultraviolet radiation source located above the quenchvessel was rotated to the vertical position.

At a time of 6 hours, the ingot was removed from the quench system usingthe titanium metal tongs and transferred to a clean radiation surfacecountertop. Exposure to external radiation sources included the metalhalide light and placement directly under a skylight (which addedfiltered sunlight to the irradiation sources). The ingot was pat dried.Upon completion of the drying, the long wave ultraviolet radiationsource located above the quench vessel was rotated vertically and movedup 1 inch. The timer was then reinitiated. The ingot was irradiated for10 minutes at which point an additional radiation source (krypton lamp)was initiated. At 12 minutes 30 seconds, the long wave ultravioletradiation source located above the quench vessel was rotated horizontaland moved down to its original position. At 13 minutes, a xenonradiation source located above the quench vessel was initiated. At 18minutes, two orthogonal fluorescent lamp racks located next to thecountertop were turned on. At 30 minutes, two angled metal halide lightslocated next to the countertop were simultaneously turned on. At thispoint the timer was again reinitiated. At 13 minutes 15 seconds, a neonradiation source located next to the countertop was turned on. At 15minutes 30 seconds, an argon radiation source located next to thecountertop was turned on. At 23 minutes 45 seconds, the argon radiationsource located next to the countertop was rotated to an angle of 35°. At37 minutes 30 seconds, the short wave ultraviolet radiation sourcelocated above the quench vessel was rotated to 35°. At 47 minutes 30seconds, the xenon radiation source located above the quench vessel wasrotated to horizontal. At 52 minutes 45 seconds, the long waveultraviolet radiation source located above the quench vessel was rotatedto 35°. At 58 minutes 30 seconds, the short wave ultraviolet radiationsource located above the quench vessel was rotated to 55°. At 77minutes, the krypton radiation source located next to the countertop wasrotated to vertical. At 89 minutes, the krypton radiation source locatednext to the countertop was rotated to 78°. At 97 minutes, the kryptonradiation source located next to the countertop was rotated to 88°.

The timer was reinitiated. At a time of 6 hours, the krypton lamp, shortwave ultraviolet, long wave ultraviolet, argon (located over quenchvessel), xenon, argon (located next to countertop), neon, two orthogonalfluorescent lamp racks, and the two angled metal halide lights weresequentially terminated in the given order. The timer was againreinitiated. At a time of 6 hours, 30 minutes, normal lab lighting(metal halides) was turned off. The timer was reinitiated. For 48 hours,the ingot was allowed to stabilize with no manual intervention (i.e., nohandling).

Example 7 Experimental Procedure for Copper, Gold, Silver, Rhenium AlloyMethod “HD” Run 14-04-03

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100 pound induction furnace reactor (Inductotherm)fitted with a 73-30R Powertrak power supply. A gas addition lance wasinstalled to a position approximately ¼ inches from the bottom of thereactor. The reactor was charged with 9080 g copper (99.98% purity), 7 grhenium, 5 g silver and 2 g gold through its charging port. The reactorwas fitted with a graphite cap and a ceramic liner (i.e., the crucible,from Engineering Ceramics). During the entire procedure, a slightpositive pressure of 97% argon, 3% hydrogen (˜0.5 psig) was maintainedin the reactor using a continuous backspace purge. Bypass injection ofgas addition was commenced (i.e., gas flow diverted around the reactorwas initiated) at a rate of 0.15 L/min of argon. The incoming gas linefor the gas addition lance passes through a sealed, light-tightenclosure whereby irradiation of the gas with precise radiation sources(e.g., wavelength, intensity, etc) can be achieved. When the entire gasline had been completely purged (assuming a plug flow model), a neonradiation source was activated within the sealed enclosure. A timer wasset to zero. Bypass flow was adjusted to 100% argon at a flow rate of0.15 L/min with trace neon present (≦0.005% vol. to ≦5%). At a time of 3minutes, an argon radiation source was activated within the sealedenclosure. After completion of another gas line purge (assuming a plugflow model), the gas line was switched from bypass to direct injectionthrough the gas addition lance.

The induction furnace power was then initiated. The reactor was heatedto 450° F., at a rate no greater than 300° F./hr, as limited by theintegrity of the crucible. The induction furnace operated in thefrequency range of 0 Hz to 3000 Hz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN3000temperature controller. Upon reaching 450° F., the gas addition lancewas repositioned to within 2 inches of the bottom of the reactor. Thetimer was again set to zero. At a time of 2 minutes, the gas compositionwas changed to 0.15 L/min of 66% nitrogen, 34% hydrogen with trace neonpresent. After completion of another gas line purge (assuming a plugflow model), a krypton radiation source is initiated in the sealedenclosure. The reactor heat up continued at a rate no greater than 300°F./hr, as limited by the integrity of the crucible, until T_(solidus)minus 30° F. was achieved. The gas flow rate was then increased to 0.3L/min with a constant gas composition. At T_(solidus) a second argonradiation source was activated within the sealed enclosure. T_(solidus)plus 8° F. was approached over a 3 to 5 minute time span. FromT_(solidus) plus 8° F. to T_(solidus) plus 15° F., the gas flow rate wasreduced to 0.15 L/min with a constant gas composition. Immediately uponreaching T_(solidus) plus 15° F., a second neon radiation source wasinitiated in the sealed enclosure. Immediately after the second neonradiation source is initiated, the gas composition is adjusted to 75%hydrogen, 22% nitrogen, and 3% argon with trace neon. The molten bathwas held at this condition for 5 minutes for stabilization.

After the 5 minute hold, the gas composition was adjusted to 20% helium,63% nitrogen, 17% argon, and trace neon. The bath was held under theseconditions for an additional 15 minutes. Again, following the hold, thegas composition and flow rate were adjusted to 100% argon with traceneon at a rate of 0.3 L/min. The reactor was held at this condition for3 minutes. The timer was reset to zero. At a time of 65 minutes,graphite saturation assemblies (⅜ inches OD, 36 inches long high purity(<5 ppm impurities) graphite rods) were inserted to the bottom of thecopper alloy charge through ports located in the top plate. The copperalloy was heated to 2359° F. over a 1 hour period. The bath was thenheld at this condition for 2 hours. Every 30 minutes during the holdperiod, an attempt was made to lower the graphite saturation assembliesas dissolution occurred. As the copper became saturated with carbon, thegraphite saturation assemblies were consumed. After the 2 hour holdperiod was complete, the graphite saturation assemblies were removed. Anadditional 2.06 grams of graphite powder was charged into the reactorthrough the charging port. The bath was then heated to 2474° F. over onehour. Upon achieving 2474° F., the gas composition and flow rate wereadjusted to 100% nitrogen with trace neon at a rate of 0.3 L/min. Holdreactor conditions for 5 minutes. The gas flow rate was reduced to 0.15L/min with constant composition. Immediately following this reduction ingas flow, the krypton radiation source in the sealed enclosure wasturned off. The timer was reset to zero. At a time of 3 minutes, the gasflow rate was reduced to 37.5 ml/min with constant composition. One ofthe argon radiation sources inside the sealed enclosure was turned off.At a time of 5 minutes, the nitrogen component of the gas flow wasdiscontinued, while maintaining the flow of trace neon. At a time of 10minutes, one of the neon radiation sources within the sealed enclosurewas rotated. The reactor temperature is lowered to 2451° F. over 7minutes.

The temperature was then varied between 2413° F. and 2451° F. for 16cycles. Each cycle consisted of raising the temperature continuouslyover 7 minutes and lowering the temperature continuously over 7 minutes.After completion of the 14.5 cycles, argon was reintroduced at a flowrate of 0.15 L/min with trace neon. Five minutes into the 15^(th) cycle,a xenon radiation source was activated within the sealed enclosure. At 6minutes into the 15^(th) cycle, a long wave ultraviolet radiation sourcewas activated in the sealed enclosure. At sweep count 15.5, a short waveultraviolet radiation source was initiated in the sealed enclosure. Atsweep count 16, the xenon radiation source was remotely rotated withinthe sealed enclosure. The temperature of the copper was varied overanother 5 cycles between 2413° F. and 2451° F. After the fifth cycle,the reactor temperature was lowered to 2400° F. over a 10 minute period.Upon achieving the target temperature of 2400, the graphite saturationassemblies were reinstalled in the copper and remained there for 1 hour.The graphite saturation assemblies were then removed.

Two voltage probes (source and ground probe) were then installed in theheadspace of the reactor and allowed to equilibrate for 5 minutes. Uponcompletion of the five minute hold the voltage probes were lowered intothe bath. The source probe was positioned 2 inches below the axialcenter and 1 inch from the radial center. The ground probe waspositioned 0.75 inches above the axial position of the source probe and1 inch from the radial center (180° from the source probe). Once theprobes were installed, a five minute hold at this condition was done toallow the bath to electronically equilibrate with the probes. Voltagewas then applied to the probes and varied between multiple voltage setpoints. This voltage application was in a continuous up/down sweepbetween two predetermined voltages. The first voltage cycle was variedbetween 17 and 18 volts for 24 cycles. Each cycle consisted of raisingthe voltage continuously over 45 seconds and lowering the voltagecontinuously over 45 seconds. The second voltage cycle was variedbetween 13.25 and 14.75 volts for 20 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The third voltage cycle was variedbetween 8.75 and 10.25 volts for 17 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The fourth voltage cycle wasvaried between 4.00 and 7.00 volts for 14 cycles. Each cycle consistedof raising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The fifth voltage cycle was variedbetween 1.50 and 5.00 volts for 10 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The sixth voltage cycle was variedbetween 0.50 and 2.00 volts for 3 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. When the final cycle was completedthe voltage was set onto a constant 1 volt setting. This voltage settingremained constant until a later step during which the leads are removed.

The reactor temperature was then lowered to 2397° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued gasaddition. The temperature was then varied between 2391° F. and 2397° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. After the 20^(th) cycle, third body gas addition waschanged by turning off the argon component of the gas leaving only traceneon gas flow. The bath was then cooled to 2388° F. over 5 minutes. Uponreaching 2388° F., one of the neon radiation sources was remotelyrotated within the sealed enclosure.

The temperature was then varied between 2380° F. and 2388° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 0.15 L/min flow of 60%argon, 40% helium, and trace neon was added, and while lowering thetemperature, a 0.3 L/min flow of 100% helium, trace neon, and tracekrypton was added. At sweep count 0.5, a krypton radiation source wasinitiated in the sealed enclosure. At sweep count 1.0, an argonradiation source was initiated in the sealed enclosure. At sweep count4.5, the short wave ultraviolet radiation source was terminated in thesealed enclosure. The reactor temperature was then lowered to 2377° F.over 5 minutes. The temperature was varied between 2346° F. and 2377° F.for 15.5 cycles. Each cycle consisted of lowering the temperaturecontinuously over 15 minutes and raising the temperature continuouslyover 15 minutes. In addition, while raising the temperature, a 0.15L/min flow of 60% argon, 40% helium, and trace neon was added, and whilelowering the temperature, a 0.3 L/min flow of 100% helium, trace neon,and trace krypton was added. After the 15.5^(th) cycle, third body gasaddition was changed by turning off all gas components except the traceneon gas flow.

After the 15.5^(th) cycle, a timer was started. At a time of 3 minutes,the xenon radiation source was remotely rotated within the sealedenclosure. The timer was then reset to zero. At 60 minutes, flow rateswere adjusted to 0.3 L/min of 100% argon and trace neon. At 65 minutes,flow rates were adjusted to 30 ml/min of 60% argon, 40% helium, andtrace neon. Immediately after the flow was adjusted, one of the neonradiation sources was remotely rotated within the sealed enclosure. At68 minutes, flow rates were adjusted to 0.15 L/min of 100% helium, traceneon, and trace krypton. At 68 minutes 20 seconds, the 1 volt power wasbrought to zero output and the voltage power leads removed from thevoltage probes. At 68 minutes 30 seconds, the long wave ultravioletradiation source was turned off in the sealed enclosure. At 71 minutes15 seconds, the voltage probes were repositioned to three inches abovethe bath surface. At 75 minutes, the source and ground probes areremoved completely from the reactor.

After the voltage probes have been removed from the reactor, flow rateswere adjusted to 0.15 L/min of 77% argon, 18% nitrogen, 5% helium andtrace neon. The reactor was then held at temperature and flow rate for15 minutes. After the 15 minute hold, one of the argon radiation sourceswas turned off in the sealed enclosure. The flow rates were immediatelyreadjusted to 0.15 L/min of 77% argon, 12% nitrogen, 11% helium andtrace neon. The reactor was then held at temperature and flow rate for25 minutes. After the 25 minute hold, the krypton radiation source wasturned off in the sealed enclosure. The flow rates were immediatelyreadjusted to 0.30 L/min of 10% argon, 90% helium and trace neon. Thereactor was then held at temperature and flow rate for 3 minutes. Afterthe 3 minute hold, flow rates were adjusted to the flow rate 0.15 L/minof 10% argon, 90% helium and trace neon and held for 2 minutes. Afterthe 2 minute hold, flow rates were adjusted to 0.30 L/min of 7%hydrogen, 93% nitrogen and trace neon and held for 10 minutes. After the10 minute hold, flow rates were adjusted to 0.15 L/min of 7% hydrogen,93% nitrogen and trace neon and held for 3 minutes. After the 3 minutehold, flow rates were adjusted to 30 ml/min of 7% hydrogen, 93% nitrogenand trace neon and held for 2 minutes. After the 2 minute hold, flowrates were adjusted to 0.15 L/min of 87% argon, 10% nitrogen, 3% heliumand trace neon and held for 5 minutes. After the 5 minute hold, flowrates were adjusted to 0.6 L/min of 90% argon, 10% nitrogen and traceneon and held for 7 minutes. After the 7 minute hold, flow rates wereadjusted to 30 ml/min of 90% argon, 10% nitrogen and trace neon and heldfor 2 minutes. After the 2 minute hold, flow rates were adjusted to 0.60L/min of 95% argon, 5% nitrogen and trace neon and held for 15 minutes.After the 15 minute hold, flow rates were adjusted to 0.30 L/min of 95%argon, 5% nitrogen and trace neon and held for 5 minutes.

The reactor temperature was then lowered to 2359° F. over 21 minutes.The temperature was then varied between 2346° F. and 2359° F. for threecycles. The cycles consisted of raising the temperature continuouslyover 27 minutes and lowering the temperature continuously over 27minutes. After the third cycle, the bath was held at 2359° F. for 5minutes. The reactor temperature was then lowered to 2346° F. over 2minutes 30 seconds. The temperature was then varied between 2359° F. and2346° F. for two cycles. The cycles consisted of raising the temperaturecontinuously over 11 minutes and lowering the temperature continuouslyover 7 minutes.

After completion of the 2^(nd) cycle, the induction power supply wasplaced into manual control. The power was then instantaneously increased5 kW above the steady state power level and immediately upon hitting the5 kW, the power was instantaneously decreased back to the steady statepower level. The power level was then varied up 3.7 kW and down 3.7 kWover 6 cycles. The cycles consisted of raising power 3.7 kW above thesteady state power level over 25 seconds. Once raised, the power levelwas held at the additional 3.7 kW setting for 45 seconds. Following the45 second hold, the power was lowered back to the steady state powerlevel over a 15 second time frame.

After the 6^(th) power cycle, the gas flows were adjusted to 0.60 L/minof 100% argon and trace neon and held for 7 minutes. Following the sevenminute hold, the argon flow was secured leaving only the trace neonflow. Once the argon flow was secured, a second lance was positionedinside the reactor. This lance was placed at a distance ⅔ from theradial center and 1.5 inches from the bottom of the bath. The centerlinelance was then repositioned to ¼ inch off the bottom. Once thecenterline lance was repositioned, flow was started in theoff-centerline lance at a rate of 30 ml/min of 100% argon and traceneon. A timer was then initiated. At a time of 2 minutes, the trace neonflow in the centerline lance was discontinued. At a time of 2 minutes 30seconds, flow was initiated in the centerline lance at a flow rate of 30ml/min of 100% carbon monoxide and held for 3 minutes. After the 3minute hold, flow rates were adjusted in the off-centerline lance to0.15 L/min of 100% argon and trace neon and held for 15 minutes. Afterthe 15 minute hold, flow rates were adjusted in the off-centerline lanceto trace neon only. Furthermore, the flow rate was adjusted in thecenterline lance to 0.60 L/min of 100% carbon monoxide and held for 10minutes. After the 10 minute hold, the carbon monoxide in the centerlinelance was turned off. The reactor temperature was then lowered toT_(solidus) plus 18° F. over 30 minutes. Upon reaching the T_(solidus)plus 18° F., flow was adjusted in the centerline lance to 0.30 L/min of100% carbon monoxide and held for 20 minutes. After the 20 minute hold,all flow was secured in the centerline lance and the lance was removed.

After the centerline lance was removed, flow rates in the off-centerlinelance were adjusted to 30 ml/min of 88% argon, 12% nitrogen and traceneon and held for 3 minutes. After the 3 minute hold, flow rates wereadjusted to 0.30 L/min of 25% helium, 75% argon and trace neon and heldfor 10 minutes. After the 10 minute hold, flow rates were adjusted to0.30 L/min of 88% argon, 12% nitrogen and trace neon and held for 10minutes. After the 10 minute hold, flow rates were adjusted to 0.15L/min of 88% argon, 12% nitrogen and trace neon and held for 5 minutes.After the 5 minute hold, flow rates were adjusted to 30 ml/min of 88%argon, 12% nitrogen and trace neon and held for 2 minutes. After the 2minute hold, flow rates were adjusted to 0.15 L/min of 88% argon, 12%nitrogen and trace neon. Once the flow rate was adjusted, the reactortemperature was lowered to T_(solidus) plus 15° F. over 45 minutes. Uponreaching the T_(solidus) plus 15° F., flow was adjusted in theoff-centerline lance to 0.30 L/min of 100% argon and trace neon and heldfor 5 minutes.

At the completion of five minute hold, the reactor temperature waslowered to T_(solidus) plus 11° F. while maintaining a temperaturelowering rate of no more than 3° F./hr. Upon reaching T_(solidus) plus11° F., flow rate in the off-centerline lance was adjusted to 0.30 L/minof 100% hydrogen and trace neon. At the completion of the flowadjustment, the reactor temperature was lowered to T_(solidus) plus 100°F. while maintaining a temperature lowering rate of no more than 3°F./hr. Upon reaching T_(solidus) plus 10° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 100% hydrogen andtrace neon. At the completion of the flow adjustment, the reactortemperature was lowered to T_(solidus) plus 9° F. while maintaining atemperature lowering rate of no more than 3° F./hr. Upon reachingT_(solidus) plus 9° F., the gas addition lance was relocated into theheadspace of the reactor, such that a quarter inch (¼ inches) dimplecould be observed on the bath surface. The bath was held at T_(solidus)plus 9° F. for an additional 5 minutes for conditioning andequilibration. The reactor was then cooled to T_(solidus) plus 8° F.while maintaining a temperature lowering rate of no more than 3° F./hr.Upon reaching T_(solidus) plus 8° F. a manual power pulse of 2 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. The reactor was then cooled to T_(solidus) plus 2° F. whilemaintaining a temperature lowering rate of no more than 3° F./hr. Uponreaching T_(solidus) plus 2° F., a manual power pulse of 1.5 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. Immediately after the 1.5 kW power pulse, flow was adjusted inthe off-centerline lance to 0.15 L/min of 50% hydrogen, 50% helium, andtrace neon. The reactor was then cooled to T_(solidus) again maintaininga temperature-lowering rate of no more than 3° F./hr. Upon reachingT_(solidus), the induction furnace power supply was lowered to 1 kW andthe reactor was allowed to cool from T_(solidus) to T_(solidus) minus75° F. Upon reaching T_(solidus) minus 75° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 60% helium, 40%hydrogen and trace neon. Following the flow adjustment, the inductionfurnace power supply was lowered to 0.75 kW and the reactor was allowedto cool to 1000° F. Upon reaching 1000° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 100% helium and traceneon. Following the flow adjustment, the induction furnace power supplywas lowered to 0.50 kW and the reactor was allowed to cool to 350° F.Upon reaching 350° F., the induction furnace power supply was shut downand a timer initiated as time zero (e.g., Timer=T₀). At a time of 5minutes, flow rate in the off-centerline lance was adjusted to 0.60L/min of 100% helium and trace neon. At a time of 9 minutes, a neonradiation source was remotely rotated within the sealed enclosure. Uponcompletion of the 90° rotation, flow in the off-centerline lance wasadjusted to 0.30 L/min of 88% argon, 12% nitrogen and trace neon.

Following the flow adjustment, the timer was reinitiated to time zero.At a time of 25 seconds, a neon radiation source within the sealedenclosure was remotely rotated. At a time of 1 minute 30 seconds, a neonradiation source within the sealed enclosure was turned off. At a timeof 5 minutes, an argon radiation source within the sealed enclosure wasturned off. At a time of 6 minute 30 seconds, flow rate was adjusted to0.30 L/min of 100% helium and trace neon. At a time of 7 minute, thesecond neon radiation source within the sealed enclosure was turned off.

The timer was reinitiated to time zero (e.g., Timer=T₀). At a time of 15minutes, the trace neon gas flow in the off-centerline lance wasstopped. At a time of 17 minutes 25 seconds, the xenon radiation sourcewas remotely rotated 90° within the sealed enclosure. At a time of 30minutes, the trace helium gas flow in the off-centerline lance wasturned off. The timer was reinitiated to time zero (e.g., Timer=T₀). Ata time of 15 minutes, the xenon radiation source inside the sealedenclosure was turned off. Thirty minutes were allowed to pass. The ingotand crucible were removed from the reactor using titanium metal tongs inthe presence of light from metal halide lamps.

Upon removal from the reactor assembly, the crucible was stripped fromthe metal ingot via a gentle wedging action. Immediately followingremoval, the ingot was transferred into a quench chamber containingdeionized water, ensuring that the top of the ingot surface was coveredby at least 6 inches of deionized (DI) water. Upon immersion into thequench chamber, a timer was established. At a time of 2 hours 15minutes, a long wave ultraviolet radiation source located above thequench vessel was initiated. At a time of 4 hours 7 minutes, a shortwave ultraviolet radiation source located above the quench vessel wasinitiated. At a time of 5 hours 59 minutes 30 seconds, the short waveultraviolet radiation source located above the quench vessel was rotatedto a vertical position.

At a time of 6 hours, the ingot was removed from the quench system usingthe titanium metal tongs and transferred to a clean radiation surfacecountertop. Exposure to external radiation sources included the metalhalide light and placement directly under a skylight (which addedfiltered sunlight to the irradiation sources). The ingot was pat dried.Upon completion of the drying, the long wave ultraviolet radiationsource located above the quench vessel was rotated to a verticalposition and moved up 1 inch. The timer was then reset to zero. Theingot was irradiated for 10 minutes at which point an additionalradiation source (krypton lamp) was initiated. At 12 minutes 30 seconds,the long wave ultraviolet radiation source located above the quenchvessel was rotated and moved down to its original position. At 13minutes, a xenon radiation source located above the quench vessel wasinitiated. At 18 minutes, two orthogonal fluorescent lamp racks locatednext to the countertop were turned on. At 30 minutes, two angled metalhalide lights located next to the countertop were simultaneously turnedon. At this point the timer was again reset. At 13 minutes 15 seconds, aneon radiation source located next to the countertop was turned on. At15 minutes 30 seconds, an argon radiation source located next to thecountertop was turned on. At 23 minutes 45 seconds, the argon radiationsource located next to the countertop was rotated to an angle of 35°. At37 minutes 30 seconds, the short wave ultraviolet radiation sourcelocated above the quench vessel was rotated to 35°. At 47 minutes 30seconds, the xenon radiation source located above the quench vessel wasrotated to horizontal. At 52 minutes 45 seconds, the long waveultraviolet radiation source located above the quench vessel was rotatedto 35°. At 58 minutes 30 seconds, the short wave ultraviolet radiationsource located above the quench vessel was rotated to 55°. At 77minutes, the krypton radiation source located next to the countertop wasrotated to vertical. At 89 minutes, the krypton radiation source locatednext to the countertop was rotated to 78°. At 93 minutes, the ingot waslifted using composite black rubber gloves and a tailored material thatacts an energy filter was placed under the ingot. The tailored materialused as an energy filter has an XRF as depicted in Appendix 1. The ingotwas then lowered onto the tailored energy filter. During theinstallation no direct skin contact with the ingot was allowed. At 97minutes, the krypton radiation source located next to the countertop wasrotated to 88°.

At this point the timer was again reset. At a time of 6 hours, thekrypton lamp, short wave ultraviolet, long wave ultraviolet, argon(located over quench vessel), xenon, argon (located next to countertop),neon, two orthogonal fluorescent lamp racks, and the two angled metalhalide lights were sequentially terminated in the given order. The timerwas again reset. At a time of 6 hours, 30 minutes, normal lab lighting(metal halides) was turned off. The timer was reset. For 48 hours, theingot was allowed to stabilize with no manual intervention (i.e., nohandling).

Example 8 Experimental Procedure for Copper Method “HD” Run 14-04-05

A cylindrical alumina-based crucible (99.68% Al₂O₃, 0.07% SiO₂, 0.08%Fe₂O₃, 0.04% CaO, 0.12% Na₂O₃; 4.5 inches O.D.×3.75 inches I.D.×14.5inches depth) of a 100 pound induction furnace reactor (Inductotherm)fitted with a 73-30R Powertrak power supply. A gas addition lance wasinstalled to a position approximately ¼ inches from the bottom of thereactor. The reactor was charged with 9080 g copper (99.98% purity)through its charging port. The reactor was fitted with a graphite capand a ceramic liner (i.e., the crucible, from Engineering Ceramics).During the entire procedure, a slight positive pressure of 97% argon, 3%hydrogen (˜0.5 psig) was maintained in the reactor using a continuousbackspace purge. Bypass injection of gas addition was commenced (i.e.,gas flow diverted around the reactor was initiated) at a rate of 0.15L/min of argon. The incoming gas line for the gas addition lance passedthrough a sealed, light-tight enclosure whereby irradiation of the gaswith precise radiation sources (e.g., wavelength, intensity, etc) wasachieved. When the entire gas line was completely purged (assuming aplug flow model), a neon radiation source was activated within thesealed enclosure. A timer was set to zero. Bypass flow was adjusted to100% argon at a flow rate of 0.15 L/min with trace neon present. (tracecan be defined as ≦0.005% vol. to ≦5%). At a time of 3 minutes, an argonradiation source was activated within the sealed enclosure. Aftercompletion of another gas line purge (assuming a plug flow model), thegas line was switched from bypass to direct injection through the gasaddition lance.

The induction furnace power was then initiated. The reactor was heatedto 450° F., at a rate no greater than 300° F./hr, as limited by theintegrity of the crucible. The induction furnace operated in thefrequency range of 0 Hz to 3000 Hz, with frequency determined by atemperature-controlled feedback loop implementing an Omega Model CN3000temperature controller. Upon reaching 450° F., the gas addition lancewas repositioned to 2 inches from the bottom of the reactor. The timerwas again set to zero. At a time of 2 minutes, the gas composition waschanged to 0.15 L/min of 66% nitrogen, 34% hydrogen with trace neonpresent. After completion of another gas line purge (assuming a plugflow model), a krypton radiation source was initiated in the sealedenclosure. The reactor heat up was continued at a rate no greater than300° F./hr, as limited by the integrity of the crucible, untilT_(solidus) minus 30° F. was achieved. The gas flow rate was thenincreased to 0.3 L/min with a constant gas composition. At T_(solidus) asecond argon radiation source was activated within the sealed enclosure.T_(solidus) plus 8° F. was approached over a 3 to 5 minute time span.From T_(solidus) plus 8° F. to T_(solidus) plus 15° F., the gas flowrate was reduced to 0.15 L/min with a constant gas composition.Immediately upon reaching T_(solidus) plus 15° F., a second neonradiation source was initiated in the sealed enclosure. Immediatelyafter the second neon radiation source was initiated, the gascomposition was adjusted to 75% hydrogen, 22% nitrogen, 3% argon andtrace neon. The molten bath was held at this condition for 5 minute forstabilization.

After the 5 minute hold, the gas composition was adjusted to 20% helium,63% nitrogen, 17% argon, and trace neon. The bath was held under theseconditions for an additional 15 minutes. Again, following the hold, thegas composition and flow rate were adjusted to 100% argon with traceneon at a rate of 0.3 L/min. The reactor was held at this condition for3 minutes. The timer was reset to zero. At a time of 65 minutes,graphite saturation assemblies (⅜ inches OD, 36 inches long high purity(<5 ppm impurities) graphite rods) were inserted to the bottom of thecopper charge through ports located in the top plate. The copper washeated to 2359° F. over a one hour period. The bath was then held atthis condition for 2 hours. Every 30 minutes during the hold period, anattempt was made to lower the graphite saturation assemblies asdissolution occurred. As the copper became saturated with carbon, thegraphite saturation assemblies were consumed. After the 2 hour holdperiod was complete, the graphite saturation assemblies were removed. Anadditional 2.06 grams of graphite powder was charged into the reactorthrough the charging port. The bath was then heated to 2474° F. over onehour. Upon achieving 2474° F., the gas composition and flow rate wereadjusted to 100% nitrogen with trace neon at a rate of 0.3 L/min. Thereactor conditions were held for 5 minutes. The gas flow rate wasreduced to 0.15 L/min with constant composition. Immediately followingthis reduction in gas flow, the krypton radiation source in the sealedenclosure was turned off. The timer was reset to zero. At a time of 3minutes, the gas flow rate was reduced to 37.5 ml/min with constantcomposition. One of the argon radiation sources inside the sealedenclosure was turned off. At a time of 5 minutes, the nitrogen componentof the gas flow was discontinued, while maintaining the flow of thetrace neon. At a time of 10 minutes, one of the neon radiation sourceswas remotely rotated (90°) within the sealed enclosure. The reactortemperature was lowered to 2451° F. over 7 minutes.

The temperature was then varied between 2413° F. and 2451° F. for 16cycles. Each cycle consisted of raising the temperature continuouslyover 7 minutes and lowering the temperature continuously over 7 minutes.After completion of the 14.5 cycles, argon was reintroduced at a flowrate of 0.15 L/min with trace neon. Five minutes into the 15^(th) cycle,a xenon radiation source was activated within the sealed enclosure. At 6minutes into the 15^(th) cycle, a long wave ultraviolet radiation sourcewas activated in the sealed enclosure. At sweep count 15.5, a short waveultraviolet radiation source was initiated in the sealed enclosure. Atsweep count 16, remotely rotate the xenon radiation source within thesealed enclosure. The temperature of the copper was varied over another5 cycles between 2413° F. and 2451° F. After the fifth cycle, thereactor temperature was lowered to 2400° F. over a 10 minute period.Upon achieving the target temperature of 2400, the graphite saturationassemblies were reinstalled in the copper and remained there for 1 hour.The graphite saturation assemblies were then removed.

Two voltage probes (source and ground probe) were then installed in theheadspace of the reactor and allowed to equilibrate for 5 minutes. Uponcompletion of the five minute hold the voltage probes were lowered intothe bath. The source probe should be positioned 2 inches below the axialcenter and 1 inch from the radial center. The ground probe waspositioned 0.75 inches above the axial position of the source probe and1 inch from the radial center (180° from the source probe). Once theprobes were installed a five minute hold at this condition was done toallow the bath to electronically equilibrate with the probes. Voltagewas then applied to the probes and varied between multiple voltage setpoints. This voltage application was in a continuous up/down sweepbetween two predetermined voltages. The first voltage cycle was variedbetween 17 and 18 volts for 24 cycles. Each cycle consisted of raisingthe voltage continuously over 45 seconds and lowering the voltagecontinuously over 45 seconds. The second voltage cycle was variedbetween 13.25 and 14.75 volts for 20 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The third voltage cycle was variedbetween 8.75 and 10.25 volts for 17 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The fourth voltage cycle wasvaried between 4.00 and 7.00 volts for 14 cycles. Each cycle consistedof raising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The fifth voltage cycle was variedbetween 1.50 and 5.00 volts for 10 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. The sixth voltage cycle was variedbetween 0.50 and 2.00 volts for 3 cycles. Each cycle consisted ofraising the voltage continuously over 45 seconds and lowering thevoltage continuously over 45 seconds. When the final cycle was completedthe voltage was set onto a constant 1 volt setting. This voltage settingremains constant until a later step during which the leads are removed.

The reactor temperature was lowered to 2397° F. over 5 minutes. Thereactor was held at this temperature for 5 minutes with continued gasaddition. The temperature was then varied between 2391° F. and 2397° F.over 20 cycles. Each cycle consisted of lowering the temperaturecontinuously over 9 minutes and raising the temperature continuouslyover 9 minutes. After the 20^(th) cycle, third body gas addition waschanged by turning of the argon component of the gas leaving only traceneon gas flow. The bath was then cooled to 2388° F. over 5 minutes. Uponreaching 2388° F., remotely rotate one of the neon radiation sourceswithin the sealed enclosure.

The temperature was then varied between 2380° F. and 2388° F. over 4.5cycles. Each cycle consisted of lowering the temperature continuouslyover 5 minutes and raising the temperature continuously over 3 minutes.In addition, while raising the temperature, a 0.15 L/min flow of 60%argon, 40% helium, and trace neon was added, and while lowering thetemperature, a 0.3 L/min flow of 100% helium, trace neon, and tracekrypton was added. At sweep count 0.5, a krypton radiation source wasinitiated in the sealed enclosure. At sweep count 1.0, an argonradiation source was initiated in the sealed enclosure. At sweep count4.5, the short wave ultraviolet radiation source was terminated in thesealed enclosure. The reactor temperature was lowered to 2377° F. over 5minute. The temperature was varied between 2346° F. and 2377° F. for15.5 cycles. Each cycle consisted of lowering the temperaturecontinuously over 15 minutes and raising the temperature continuouslyover 15 minutes. In addition, while raising the temperature, a 0.15L/min flow of 60% argon, 40% helium, and trace neon was added, and whilelowering the temperature, a 0.3 L/min flow of 100% helium, trace neon,and trace krypton was added. After the 15.5^(th) cycle, third body gasaddition was changed by turning off all gas components except the traceneon gas flow.

After the 15.5^(th) cycle, a timer was established. At a time of 3minutes, the xenon radiation source was rotated 90° within the sealedenclosure. The timer was then reset to zero. At 60 minutes, flow rateswere adjusted to 0.3 L/min of 100% argon and trace neon. At 65 minutes,flow rates were adjusted to 30 ml/min of 60% argon, 40% helium, andtrace neon. Immediately after the flow was adjusted, one of the neonradiation sources was remotely rotated 90° within the sealed enclosure.At 68 minutes, flow rates were adjusted to 0.15 L/min of 100% helium,trace neon and trace krypton. At 68 minutes 20 seconds, the 1 volt powerwas brought to zero output and the voltage power leads removed from thevoltage probes. At 68 minutes 30 seconds, the long wave ultravioletradiation source was turned off in the sealed enclosure. At 71 minutes15 seconds, the voltage probes were repositioned to three inches abovethe bath surface. At 75 minutes, the source and ground probes wereremoved completely from the reactor.

After the voltage probes had been removed from the reactor, flow rateswere adjusted to 0.15 L/min of 77% argon, 18% nitrogen, 5% helium andtrace neon. The reactor was then held at temperature and flow rate for15 minutes. After the 15 minute hold, an argon radiation source wasturned off in the sealed enclosure. The flow rates were immediatelyreadjusted to 0.15 L/min of 77% argon, 12% nitrogen, 11% helium andtrace neon. The reactor was then held at temperature and flow rate for25 minutes. After the 25 minute hold, the krypton radiation source wasturned off in the sealed enclosure. The flow rates were immediatelyreadjusted to 0.30 L/min of 10% argon, 90% helium and trace neon. Thereactor was then held at temperature and flow rate for 3 minutes. Afterthis 3 minute hold, flow rates were adjusted to 0.15 L/min of 10% argon,90% helium and trace neon and held for 2 minutes. After this 2 minutehold, flow rates were adjusted to 0.30 L/min of 7% hydrogen, 93%nitrogen and trace neon and held for 10 minutes. After this 10 minutehold, flow rates were adjusted to 0.15 L/min of 7% hydrogen, 93%nitrogen and trace neon and held for 3 minutes. After this 3 minutehold, flow rates were adjusted to 30 ml/min of 7% hydrogen, 93% nitrogenand trace neon and held for 2 minutes. After this 2 minute hold, flowrates were adjusted to 0.15 L/min of 87% argon, 10% nitrogen, 3% heliumand trace neon and held for 5 minutes. After this 5 minute hold, flowrates were adjusted to 0.6 L/min of 90% argon, 10% nitrogen and traceneon and held for 7 minutes. After this 7 minute hold, flow rates wereadjusted to 30 ml/min of 90% argon, 10% nitrogen and trace neon and heldfor 2 minutes. After this 2 minute hold, flow rates were adjusted to0.60 L/min of 95% argon, 5% nitrogen and trace neon and held for 15minutes. After this 15 minute hold, flow rates were adjusted to 0.30L/min of 95% argon, 5% nitrogen and trace neon and held for 5 minutes.

The reactor temperature was then lowered to 2359° F. over 21 minutes.The temperature was then varied between 2346° F. and 2359° F. for threecycles. The cycles consisted of raising the temperature continuouslyover 27 minutes and lowering the temperature continuously over 27minutes. After the third cycle, the bath was held at 2359° F. for 5minutes. The reactor temperature was then lowered to 2346° F. over 2minutes 30 seconds. The temperature was then varied between 2359° F. and2346° F. for two cycles. The cycles consisted of raising the temperaturecontinuously over 11 minutes and lowering the temperature continuouslyover 7 minutes.

After the completion of the 2^(nd) cycle, the induction power supply wasplaced into manual control. The power was then instantaneously increased5 kW above the steady state power level and immediately upon hitting the5 kW increase the power was instantaneously decreased back to the steadystate power level. The power level was then varied up 3.7 kW and down3.7 kW over 6 cycles. The cycles consisted of raising power 3.7 kW abovethe steady state power level over 25 seconds. Once raised, the powerlevel was held at the additional 3.7 kW setting for 45 seconds.Following the 45 second hold, the power was lowered back to the steadystate power level over a 15 second time frame.

After the 6^(th) power cycle, the gas flows were adjusted to 0.60 L/minof 100% argon and trace neon and held for 7 minutes. Following the sevenminute hold, the argon flow was turned off leaving only the trace neonflow. Once the argon flow was turned off, a second lance was positionedinside the reactor. This lance should be placed at a position ⅔ of thedistance from the radial center and 1.5 inches from the bottom of thebath. The centerline lance was then repositioned to ¼ inch from thebottom. Once the centerline lance was repositioned, flow was started inthe off-centerline lance at a rate of 30 ml/min of 100% argon and traceneon. A timer was then initiated at zero (e.g., Timer=T₀). At a time of2 minutes, the trace neon flow in the centerline lance was stopped. At atime of 2 minutes 30 seconds, flow was initiated in the centerline lanceat a flow rate of 30 ml/min of 100% carbon monoxide and held for 3minutes. After the 3 minute hold, flow rates were adjusted in theoff-centerline lance to 0.15 L/min of 100% argon and trace neon and heldfor 15 minutes. After the 15 minute hold, flow rates were adjusted inthe off-centerline lance to trace neon only. Furthermore, the flow ratewas adjusted in the centerline lance to 0.60 L/min of 100% carbonmonoxide and held for 10 minutes. After the 10 minute hold, the carbonmonoxide in the centerline lance was turned off. The reactor temperaturewas then lowered to T_(solidus) plus 18° F. over 30 minutes. Uponreaching the T_(solidus) plus 18° F., flow was adjusted in thecenterline lance to 0.30 L/min of 100% carbon monoxide and held for 20minutes. After the 20 minute hold, all flow was discontinued in thecenterline lance and the lance was removed.

After the centerline lance was removed, flow rates are adjusted in theoff-centerline lance to 30 ml/min of 88% argon, 12% nitrogen and traceneon and held for 3 minutes. After the 3 minute hold, flow rates wereadjusted to 0.30 L/min of 25% helium, 75% argon and trace neon and heldfor 10 minutes. After the 10 minute hold, flow rates were adjusted to0.30 L/min of 88% argon, 12% nitrogen and trace neon and held for 10minutes. After the 10 minute hold, flow rates were adjusted to 0.15L/min of 88% argon, 12% nitrogen and trace neon and held for 5 minutes.After the 5 minute hold, flow rates were adjusted to 30 ml/min of 88%argon, 12% nitrogen and trace neon and held for 2 minutes. After the 2minute hold, flow rates were adjusted to 0.15 L/min of 88% argon, 12%nitrogen and trace neon. Once the flow rate was adjusted, the reactortemperature was then lowered to T_(solidus) plus 15° F. over 45 minutes.Upon reaching the T_(solidus) plus 15° F., flow was adjusted in theoff-centerline lance to 0.30 L/min of 100% argon and trace neon and heldfor 5 minutes.

At the completion of the 5 minute hold, the reactor temperature was thenlowered to T_(solidus) plus 11° F. while maintaining a temperaturelowering rate of no more than 3° F./hr. Upon reaching T_(solidus) plus11° F., the flow rate in the off-centerline lance was adjusted to 0.30L/min of 100% hydrogen and trace neon. At the completion of the flowadjustment, the reactor temperature was then lowered to T_(solidus) plus10° F. while maintaining a temperature lowering rate of no more than 3°F./hr. Upon reaching T_(solidus) plus 10° F., the flow rate in theoff-centerline lance was adjusted to 30 ml/min of 100% hydrogen andtrace neon. At the completion of the flow adjustment, the reactortemperature was lowered to T_(solidus) plus 9° F. while maintaining atemperature lowering rate of no more than 3° F./hr. Upon reachingT_(solidus) plus 9° F., the gas addition lance was relocated into theheadspace of the reactor, such that a quarter inch (¼ inches) dimplecould be observed on the bath surface. The bath was held at T_(solidus)plus 9° F. for an additional 5 minutes for conditioning andequilibration. The reactor was then cooled to T_(solidus) plus 8° F.while maintaining a temperature lowering rate of no more than 3° F./hr.Upon reaching T_(solidus) plus 8° F. a manual power pulse of 2 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. The reactor was then cooled to T_(solidus) plus 2° F. whilemaintaining a temperature lowering rate of no more than 3° F./hr. Uponreaching T_(solidus) plus 2° F. a manual power pulse of 1.5 kW wasintroduced with a single continuous up/down sweep from normal holdingpower. Immediately after the 1.5 kW power pulse, flow was adjusted inthe off-centerline lance to 0.15 L/min of 50% hydrogen, 50% helium andtrace neon. The reactor was then cooled to T_(solidus) again maintaininga temperature-lowering rate of no more than 3° F./hr. Upon reachingT_(solidus) the induction furnace power supply was lowered to 1 kW andthe reactor was allowed to cool from T_(solidus) to T_(solidus) minus75° F. Upon reaching T_(solidus) minus 75° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 60% helium, 40%hydrogen and trace neon. Following the flow adjustment, the inductionfurnace power supply was lowered to 0.75 kW and the reactor was allowedto cool to 1000° F. Upon reaching 1000° F., flow rate in theoff-centerline lance was adjusted to 30 ml/min of 100% helium and traceneon. Following the flow adjustment, the induction furnace power supplywas lowered to 0.50 kW and the reactor was allowed to cool to 350° F.Upon reaching 350° F., the induction furnace power supply was shut downand a timer initiated at time zero. At a time of 5 minutes, flow rate inthe off-centerline lance was adjusted to 0.60 L/min of 100% helium andtrace neon. At a time of 9 minutes, a neon radiation source within thesealed enclosure was remotely rotated 90°. Upon completion of therotation, flow in the off-centerline lance was adjusted to 0.30 L/min of88% argon, 12% nitrogen and trace neon.

Following the flow adjustment, reinitiate the timer to zero. At a timeof 25 seconds, remotely rotate a neon radiation source within the sealedenclosure (90°). At a time of 1 minute 30 seconds, a neon radiationsource within the sealed enclosure was turned off. At a time of 5minutes, a argon radiation source within the sealed enclosure was turnedoff. At a time of 6 minute 30 seconds, flow rate was adjusted to 0.30L/min of 100% helium and trace neon. At a time of 7 minute, the secondneon radiation source within the sealed enclosure was turned off.

The timer was reinitiated to time zero. At a time of 15 minutes, thetrace neon gas flow in the off-centerline lance was turned off. At atime of 17 minutes 25 seconds, the xenon radiation source within thesealed enclosure was remotely rotated 90°. At a time of 30 minutes, thetrace helium gas flow in the off-centerline lance was turned off. Thetimer was reinitiated to time zero. At a time of 15 minutes, the xenonradiation source inside the sealed enclosure was turned off. Thirtyminutes were allowed to pass. The ingot and crucible were removed fromthe reactor in the presence of radiation sources (metal halide lightsources) utilizing titanium metal tongs.

Upon removal, the crucible was stripped from the metal ingot via agentle wedging action. Immediately following removal, the ingot wastransferred into a quench chamber containing deionized water, ensuringthat the top of the ingot surface was covered by at least 6 inches of DIwater. Upon entrance into the quench chamber, a timer was established attime zero. At a time of 2 hours 15 minutes, a long wave ultravioletradiation source located above the quench vessel was initiated. At atime of 4 hours 7 minutes, a short wave ultraviolet radiation sourcelocated above the quench vessel was initiated. At a time of 5 hours 59minutes 30 seconds, the short wave ultraviolet radiation source locatedabove the quench vessel was rotated (90°) to a tip up position.

At a time of 6 hours, the ingot was removed from the quench system usingthe titanium metal tongs and transferred to a clean radiation surfacecountertop. Exposure to external radiation sources included the metalhalide light and placement directly under a skylight (which addedfiltered sunlight to the irradiation sources). The ingot was pat dried.Upon completion of the drying, the long wave ultraviolet radiationsource located above the quench vessel was rotated to a verticalorientation and moved up 1 inch. The timer was then reset to zero. Theingot was irradiated for 10 minutes at which point an additionalradiation source (krypton lamp) was initiated. At 12 minutes 30 seconds,the long wave ultraviolet radiation source located above the quenchvessel was rotated (90°) and moved down to its original position. At 13minutes, a xenon radiation source located above the quench vessel wasinitiated. At 18 minutes, two orthogonal fluorescent lamp racks locatednext to the countertop were turned on. At 30 minutes, two angled metalhalide lights located next to the countertop were simultaneously turnedon. At this point the timer was again reset to zero. At 13 minutes 15seconds, a neon radiation source located next to the countertop wasturned on. At 15 minutes 30 seconds, an argon radiation source locatednext to the countertop was turned on. At 23 minutes 45 seconds, theargon radiation source located next to the countertop was rotated to anangle of 35°. At 37 minutes 30 seconds, rotate the short waveultraviolet radiation source located above the quench vessel to 35°. At47 minutes 30 seconds, the xenon radiation source located above thequench vessel was rotated to a horizontal orientation. At 52 minutes 45seconds, the long wave ultraviolet radiation source located above thequench vessel was rotated to 350. At 58 minutes 30 seconds, the shortwave ultraviolet radiation source located above the quench vessel wasrotated to 55°. At 77 minutes, the krypton radiation source located nextto the countertop was rotated to a vertical orientation. At 89 minutes,the krypton radiation source located next to the countertop was rotatedto 78°. At 93 minutes, the ingot was lifted using composite black rubbergloves and a tailored material that acts as an energy filter was placedunder the ingot. The tailored material used as an energy filter has anXRF as depicted in Appendix 1. The ingot was then lowered onto thetailored energy filter. At 97 minutes, the krypton radiation sourcelocated next to the countertop was rotated to 88°.

At this point the timer was again reset to zero. At a time of 6 hours,the krypton lamp, short wave ultraviolet, long wave ultraviolet, argon(located over quench vessel), xenon, argon (located next to countertop),neon, two orthogonal fluorescent lamp racks, and the two angled metalhalide lights were sequentially turned off in the given (aforementioned)order. The timer was again reset to zero. At a time of 6 hours, 30minutes, normal lab lighting (metal halides) was turned off. The timerwas reset to zero. For 48 hours, the ingot was allowed to stabilize withno manual intervention (i.e., no handling).

Analytical Protocols:

X-Ray Fluorescence

An ARL 8410 XRF was used to analyze each of the sample ingots. An ARL8410 is a sequential wavelength dispersive spectrometer (WDS). Specificemission lines are used to determine the presence or absence, and theconcentrations of various elements. Each characteristic x-ray line ismeasured in sequence by the instrument by controlling the instrumentgeometry.

The ARL 8410 (WDS) spectrometer relies on the fundamentals of x-raydiffraction. X-ray fluorescence occurs when matter is bombarded by astream of high-energy incident x-ray photons. When the incidentX-radiation strikes the sample, the incident x-rays may be absorbed,scattered, or transmitted for the measurement of the fluorescent yield.

The ARL 8410 utilizes an end-window rhodium (Rh) x-ray tube. Theend-window is composed of beryllium, and holds the tube at high vacuum.The filaments are heated giving off electrons by thermoionic emission.This beam of electrons then bombards the target Rh anode across a 10-70keV voltage potential. Thus, primary x-rays are produced during thecollision. The emitted x-ray spectrum consists of (1) “Continuum” or“Bremstrahlung” radiation, (2) Characteristic x-ray lines of the targetmaterial (e.g., K and L series), and (3) Characteristic lines from anycontaminants. Thus, the primary spectrum appears as a series of sharpintense peaks arrayed over a broad hump of continuum radiation. The ARLis equipped with and uses two types of photon detectors, the FlowProportional Counter (FPC) and the Scintillation Counter (SC).

The manufactured metal samples, unless otherwise specified, are preparedby cutting a sample with an approximate cross-section of 1.1875″ fromthe cooled ingot. The axial edge and radial edge are then denoted. Fornon-brittle samples, a cube-shaped sample is used. When possible, asmooth surface is prepared for analysis; the axial and radial faces aresequentially polished. The sample faces are sanded to 400 grit and thena polishing wheel is employed with 600 grit paper. Finally, a 1 μmpolishing compound completes the smoothing process.

Prior to analysis, the sample is cleaned with isopropyl alcohol (IPA)and placed in a sample cassette/holder. The sample holder is then loadedinto the XRF.

The orientation of the detector crystal with respect to the sample andthe photon detector is controlled synchronously such that characteristicx-ray lines can be accurately measured. A sequential measurementconsists of positioning the diffraction crystal at a given theta(diffraction angle) and the detector at two-theta and counting for agiven period of time. The crystal and detector are then rotated to adifferent angle for the next characteristic x-ray line.

XRF 386 Software by Fisons Instruments is used to control the crystaland detector placement. Uniquant Version 2 software, developed by OmegaData Systems provides the data reduction algorithms for each analyticalprotocol. The sample results include an elemental composition list alongwith the associated concentrations for each sample.

Measurement of Magnetism and Material Attraction

The magnetic and material attraction properties of the manufacturedingots were tested via four methods:

Magnetic Attraction: An ⅛ inch diameter (0.0625 inch thick) neodymiumiron boron magnet (NdFeB) was scanned consistently and uniformly acrossthe surface of the ingot to detect areas of attraction. Areas ofattraction were then noted at specific sites on the surface in both avertical and horizontally inverted (i.e., upside down) orientation.Attraction to Iron: The attraction of iron chips (99%_(wt) purity;between 10 and 25 mesh), iron powder (94%_(wt) Fe, 3%_(wt) C, 3%_(wt)S), and spherical sponge iron (99.8%_(wt) purity, ⁻50 to ⁺100 mesh) tospecific areas on the tailored ingots was observed and recorded. Theretention of the iron media (chips, sponge balls, or powder) on theingot surface was observed in a vertical and horizontally inverted(i.e., upside-down) orientation.Gauss Measurement: An F. W. Bell 4048 Gauss meter was used to performprecise measurements of the magnetic fields observable across thesurfaces of the ingots. A scan of each face was performed to creategrids of the magnetic force. These scans provide an indication of themagnetic flux density, the property of magnetic fields that determinesthe force that is exerted upon a current or moving charge. Hence, alarge magnetic field measurement should be indicative of strongattraction and conversely no magnetic field measurement should beindicative of no attraction. The magnetic behavior of various points onthe ingot were specifically quantified to note that even though theyexhibited clear magnetic attraction, an insignificant Gauss reading wasobserved (e.g., comparable to the background magnetic field measured atthe earth's surface).Non-magnetic Attraction: Many of the manufactured materials were foundto exhibit unique attraction to non-magnetic, non-ferromagneticmaterials. For example, sulfur powder was shown to exhibit an attractionto the surface of the tailored ingots. The sulfur powder (99.9% purity,20 mesh) was spread evenly over the surface of the clean, polished, drymanufactured ingot. The ingot was then rotated to a vertical position(90° to the ground). The retention of powder was documented viaphotography and manual mapping in a lab notebook. The sample wasinverted completely (180° rotation from its resting position on thesurface). Again, powder retention was documented. This procedure wasrepeated on both the top and bottom surfaces of the manufactured ingot.Hardness

Hardness testing was performed via multiple techniques, including Moh'shardness testing and Rockwell hardness testing (both standardtechniques). In Moh's hardness testing the test angle approaches 0°,while in Rockwell testing the test angle approaches 90°. By testing atmultiple angles, changes to different contributing aspects of changingthe composition of matter could be tested.

The Rockwell method (ASTM 18-84 Standard Test Methods for RockwellHardness and Rockwell Superficial Hardness of Metallic Materials)employs either a ball or a diamond cone in a precision-testinginstrument that is designed to measure depth of penetration accurately.Two superimposed impressions are made, one with a load of 10 kg and thesecond with a load of 100 kg. The depth to which the major load drivesthe ball or cone below that depth to which the minor load has previouslydriven it is taken as a measure of the hardness. For hardened steels,greater accuracy is obtained by using a diamond cone (120° with slightlyrounded tip) applied under a major load of 150 kg. The Rockwell hardnesstest B uses the 1/16″ diameter steel ball with a 100 kg load. Scale B isappropriate for copper alloys, soft steels, aluminum alloys, malleableiron, etc.; Scale C is appropriate for steel, hard cast irons, pearliticmalleable iron, titanium, deep case hardened steel and other materialsharder than B 100. The method using the cone is designated Rockwell Ctest. Based on the depth of the indentation, the hardness scale can beread directly from the scale, the higher the number, the harder thematerial. The dial-like scale is really a depth gauge, graduated inspecial units specific to the test being performed, e.g., RockwellHardness C.

The Rockwell results are a useful measure of relative resistance toindentation; however, the Rockwell test does not serve well as apredictor of other properties such as strength or resistance toscratches, abrasion, or wear. Hence, the Rockwell hardness test cannotbe used alone for product specifications.

The Moh's Scales, in use since 1822, is used to rank the relativehardness of minerals via the ability of materials to resist scratchingby another material. Moh's scale consists of 10 minerals arranged inorder from 1 to 10. Diamond is rated as the hardest and is indexed as10. Talc is indexed as 1 and is the softest. Each mineral in the scalewill scratch those below it:

Mineral Index Diamond 10 Corundum 9 Topaz 8 Quartz 7 Orthoclase(Feldspar) 6 Apatite 5 Fluorite 4 Calcite 3 Gypsum 2 Talc 1The steps are not of equal value (i.e., nonlinear) and the difference inhardness between 9 and 10 is much greater than between 1 and 2 (i.e.,step size approaches an exponential function). The hardness isdetermined by finding which of the standard minerals the test materialwill scratch or not scratch; the hardness will lie between two points onthe scale—the first point being the mineral which is scratched and thenext point being the mineral which is not scratched. In thedetermination procedure, it is necessary to be certain that a scratch isactually made and not just a “chalk” mark that will rub off. Naturalcopper is between 2 and 3 and tool steel is between 6 and 7.Appearance/Color

The color of each sample is noted via visual evaluation. In addition,unique surface configurations are documented (for example, the expulsionof material from the bath upon cooling). Digital photography is used todocument the physical appearance.

Results:

The following is a list of manufactured materials prepared by thetechniques described herein and the ingot compositions.

TABLE 1 Manufactured Ingots Prepared via Specified TechniqueExperimental Experimental Quantity Purity Protocol/Method Run NumberMetal (grams) (wt %) “AB” 14-03-02 Copper 9080 99.98 (Example 1) “AB”without 14-03-03 Copper 9080 99.98 EM radiation “AB” 14-01-10 Aluminum3454 99.9 “AB” 14-01-11 Aluminum 3454 99.9 “HA” 14-02-06 Copper 908099.98 (Example 2) “HA” 14-04-02 Aluminum 4540 99.99 (Example 3) “HD”14-01-20 Cobalt 8899 99.5 (Example 4) Vanadium 182 99.5 Rhenium 7 99.997“HD” 14-01-21 Nickel 9080 99.97 (Example 5) Rhenium 5 99.997 “HD”14-01-13 Iron 8534 99.98 (Example 6) Vanadium 182 99.5 Chromium 18299.999 Manganese 182 99.99 “HD” 14-04-03 Copper 9080 99.98 (Example 7)Rhenium 7 99.997 Silver 5 99.99 Gold 2 99.99 “HD” 14-04-05 Copper 908099.98 (Example 8) “HD” with 14-01-15 Iron 8534 99.98 modulated coolVanadium 182 99.5 down Chromium 182 99.999 Manganese 182 99.99 “HD” with14-02-03 Iron 9973.4 99.98 modulated EM Vanadium 212.2 99.5 radiationChromium 212.2 99.999 Manganese 212.2 99.99 “HD” with 14-04-06 Copper9080 99.98 modulated (EM radiation) angle of incidenceXRF Results:

Appendix 2 shows tables of XRF data results for the manufacturedmaterials. Note in each table the apparent detection of materials notpresent in the initial starting materials. Such detections areindicative of a shift in the energy of the manufactured materials,manifesting itself in “false positives” for the detection of elementsnot present.

In addition, despite the fact that the manufactured ingots were preparedin a very well-mixed reactor, where composition should be homogeneous,significant “apparent” compositional differences exist in the axial andradial directions. Note XRF data for each ingot is presented inback-to-back tables in Appendix 2. This anisotropic behavior is againindicative of changes in the energy patterning of the manufacturedmaterials.

Such shifts in energy are demonstrated best in identical experimentsthat were performed manufacturing copper (Runs 14-03-02 and 14-03-03).The primary difference in these two experimental runs was to performelectromagnetic (EM) energy addition to the third-body gases prior toinjection into the reactor. The XRF results for these experiments aresummarized below in Table 2:

TABLE 2 XRF Results Summary for 14-03-02 and 14-03-03 14-03-02 (EMradiation addition Element through third-body gases) 14-03-03 (wt %)Axial Radial Axial Radial Cu 97.95 99.03 99.55 99.23 Al 1.79 0.79 0.230.29 Si 0.111 — 0.038 0.27 La 0.012 — 0.02 — Pr 0.005 — — 0.006 Gd — —0.003 0.003 Er — 0.008 0.013 0.017 ΣConc. 99.8 99.5 99.0 99.3Note the differences in axial and radial concentrations; the detectionof elements not present in any of the initial feed materials or reactormaterials; and the differences in experimental results for identicalexperimental programs except for the addition of EM radiation throughthird-body gases.Physical Appearance and Color

Visual inspection of the manufactured materials indicates that thephysical characteristics of the material have been dramatically altered.Major physical changes can include color, texture, the appearance ofvoid spaces in the ingot internals, the expulsion of metal during thecooling process, and apparent volumetric changes.

Comparison of ingots of similar composition, but manufactured viaalternate techniques, can exemplify the physical manifestations ofchanges to the composition of matter. The exterior volume of ingot14-04-01 (Example 1 of U.S. Ser. No. 10/123,028, substituting Al for Cu)is significantly greater (˜30%) than 14-04-02 with an internal void inthe ingot that runs approximately 80% down the length of the ingot.Interestingly, the ingot 14-04-01 was subjected to lower volumetric gasflow rates than ingot 14-04-02; hence gas expansion is not a plausibleexplanation for the physical differences. Additionally, the ingotprepared via the subject method exhibits a definite charcoal appearance,as opposed to the silvery appearance of 14-04-01. The exteriors are alsodifferent: smooth versus foil-like. Note that the magnetic behavior ofingot 14-04-01 was stronger than that of 14-04-02; yet both exhibitedmagnetic behavior not seen in natural aluminum. See magnetic attractionsection for a discussion of magnetic attraction in tailored materials.

Similar differences in physical appearance were observed in manufacturedcopper ingots as well. The observed physical differences between the twoingots were:

-   -   14-01-01 (Example 1 of U.S. Ser. No. 10/123,028) had a void        running approximately ⅓-½ the depth of the ingot; while 14-02-06        actually had major expulsion of material from the bath.    -   14-01-01 had the traditional copper color with some iridescence        while the ingot 14-02-06 exhibited a strong red color, also with        some iridescence and apparent band gap shift.

Interesting physical characteristics were also observable in copperingots prepared by one of the alternate techniques described herein.Based on alterations to the experimental plan, for example changes tothe third body addition and/or electromagnetic radiation sources, thematerial outcome were significantly different.

Two copper ingots developed via an identical experimental plan exceptfor the addition of electromagnetic radiation through third-bodyaddition. The surface of ingot 14-03-02 was smooth and exhibits whatcould be described as a “wood grain” finish. Ingot 14-03-03 exhibited a“dimpled” rough finish, with what appeared to be mosaic patterning.Material expulsion to form a “crown” was also more significant in run14-03-03. The color in ingot 14-03-02 followed the traditional coppercoloring more closely than 14-03-03 that exhibited a broader spectrum ofcolors including red and brown tones. As Table 2 shows, the inducedelements were different for the two runs despite being prepared in thesame containment system, with identical operating conditions except forthe addition of EM radiation to third body gases. Hence, the compositionof matter has clearly been altered in both of these manufactured ingots.

Hardness Testing

Hardness testing was performed on material standards, natural copper,manufactured copper prepared via the technique outlined in U.S. Pat. No.6,572,792 B 1, and manufactured copper prepared by the techniquedelineated herein. Two primary hardness techniques were used: RockwellHardness and Moh's Hardness.

The Metals Handbook defines hardness as “Resistance of metal to plasticdeformation, usually by indentation.” However, the term may also referto stiffness or temper, to resistance to scratching, abrasion, orcutting. Hardness testing does not give a direct measurement of anengineering performance property; it correlates well with strength, wearresistance, and other properties.

Rockwell Hardness testing is an indentation testing method in which anindenter is impressed into the test sample at a prescribed load tomeasure the material's resistance to deformation. A Rockwell hardnessnumber is then calculated from the depth of permanent deformation of thesample after application and removal of the test load. Various indentershapes and sizes combined with a range of test loads form a matrix ofRockwell hardness scales.

Moh's Hardness testing is a scratch test in which known standards areused to scratch materials to specify surface hardness through resistanceto scratching. Interesting test results were obtained in the testing ofmany of the manufactured ingots. For example, a sample could exhibit anexceptionally high Moh's hardness (i.e., resistance to scratchingindicative of strong interfacial energy enhancement) yet shatter underthe Rockwell Hardness Test (i.e., highly brittle material).

A Moh's scratch test was performed on a manufactured Fe/V/Cr/Mn ingot.The surface was impervious to scratching by the Moh's Standard for ahardness of 10, diamond. In fact, the diamond tip was actually damagedby the manufactured alloy, indicating that the tailored material had anapparent Moh's Hardness >10. Tool steel, a man-made material of naturalelements with a similar composition to this tailored ingot, typicallyhas a Moh's hardness between 6 and 7. This tailored material exhibited ahardness far exceeding that which would be expected from naturalmaterials and greater than that which had been seen in any previousmanufactured material (i.e., materials prepared via the method presentedin U.S. Pat. No. 6,572,792). Quite clearly, this process for tailoringmaterial can significantly raise the hardness, with an abundance ofbeneficial, commercially-relevant implications (e.g., drilling, mining,etc.).

Similar results on another tailored copper ingot compared with somestandards provided by the testing manufacturer. Note that the tailoredmaterial exhibited a very high Moh's hardness factor and exhibitedgreater hardness in the radial direction than in the axial direction.This anisotropic hardness behavior is generated through materialtailoring. Despite this Moh's hardness factor, the same tailored ingotexhibited brittle failure during the Rockwell testing.

Magnetic and Material Attraction

Three different copper ingots were tailored via the techniques describedherein. Each of these ingots was subjected to a slightly differentexperimental protocol. For example, the experimental program may havevaried by the time, type, or method of EM radiation addition. Theresultant magnetic and physical attraction properties of each ingot aresignificantly different from natural copper and significantly differentfrom each other. The attraction behavior of these three ingots issummarized in below:

TABLE 3 Attraction Behavior of Tailored Copper Ingots (9080 g, 99.98%purity) NdFeB Experimental Experimental Magnet Sulfur Run NumberProtocol/Method Attraction Attraction 14-02-06 “HA” Observed Observed14-04-05 “HD” Observed Observed 14-03-02 “AB” Observed Observed NaturalCopper None None

Each ingot exemplified magnetic attraction induced by the tailoringprocess: behavior not present in natural copper. In addition to magneticattraction, these ingots exhibited attraction to other non-magneticmaterials, such as sulfur. In each case, the testing for the attractionbehavior of the sulfur powder was performed on a clean, polished, drysurface of the ingot to prohibit any effects of surface tension oradhesion. Additionally, the areas of magnetic attraction and sulfurattraction were at significantly different locations on the ingot,removing the possibility of induced attraction or other extraneoussurface effects.

Three important points to note:

-   -   1. The sulfur attraction was at different locations than the        magnetic attraction, eliminating induction, surface        irregularities, surface adhesion, etc. as possible explanations        for the attraction.    -   2. The intensity of the sulfur attraction and the magnetic        attraction mimicked each other. That is, ingots that exhibit        multiple points of magnetic attraction (widespread) tend to have        extensive regions of sulfur attraction.    -   3. The surfaces were polished, cleaned, and dried thoroughly        before the testing was performed. Analysis was performed in a        fully vertical position.

Each of these points supports the supposition of a change in thecomposition of matter affecting the electromagnetic behavior of thetailored material. Natural copper exhibits no attraction to eithermagnets or sulfur. Yet, the manufactured copper, tailored via threedifferent protocols, all exhibited unique attraction behavior.

In addition to pure copper, various alloys were subjected to theexperimental protocol outlined herein and similar results were obtained:non-ferromagnetic material attraction, ferromagnetic materialattraction, and magnetic attraction.

The first example of such behavior is a Nickel/Rhenium ingot, Ingot14-01-21. This ingot, composed predominantly of Ni, will attract amagnet in its natural state. Hence, no magnetic testing was performed.However the attraction of sulfur powder and various ferromagneticmaterials (Fe chips (99%_(wt) purity; 10-25 mesh), spherical sponge Fe(ranging from ⁻50 to ⁺100 mesh, 99.8%_(wt) pure), and Fe powder 94%_(wt)Fe, 3%_(wt) S, and 3%_(wt) C, none of which are attracted to naturalnickel or rhenium in the absence of an induced magnetic field caused bythe presence of a magnet) were tested.

The Nickel/Rhenium tailored ingot exhibited unique material attractionthroughout the entire ingot (i.e., a volumetric property vs. a surfaceproperty) as exemplified on multiple faces of the cut ingot. To furtherdemonstrate that surface irregularities are not the source of the uniqueattraction, an ingot was cut and the surface polished. The clean, dry,polished surface was then used for evaluating the attraction behavior oftailored materials.

In a similar emulation of the behavior observed in the tailored copperingots, the tailored Nickel/Rhenium ingot also exhibited significantattraction to sulfur powder.

To further demonstrate that the attraction behavior is caused by achange in the composition of matter that in turn alters theelectromagnetic behavior of the tailored material, a polished surface ofthe Ni/Re tailored ingot was tested for sulfur attraction (i.e.,eliminate the effects of surface irregularities). Additionally, theingot was rotated 180°. The same attraction patterning was observedindependent of vertical orientation, eliminating a surface lip or defectas a possible explanation for the attraction.

To demonstrate that the attraction behavior observed was not unique tonickel alloys (e.g., due to their ferromagnetic behavior), a similar setof attraction experiments was performed on a tailored copper ingotcontaining Cu, Re, Ag, and Au. Sulfur attraction was achieved onmultiple surfaces, in this instance, the top and the bottom.

This tailored copper alloy ingot exhibited multiple points of attractionto a Nd/Fe/B magnet.

In yet another set of experiments to investigate the behavior oftailored ingots that are ferromagnetic in their natural state (i.e., canbe induced to have a magnetic field, through the alignment of magneticmoments using a natural magnet), a tailored cobalt alloy ingot (Co/V/ReIngot 14-01-20) was tested for material attraction immediately followingthe end of the tailoring process. The manufactured Co/V/Re ingot didattract iron immediately following the tailoring process in limitedregions.

Given these positive attraction-testing results, further tests wereperformed on the tailored copper and copper alloy (non-ferromagnetic)ingots. These non-ferromagnetic materials should not attract either amagnet or iron in their natural state. Yet, each of the manufacturedcopper ingots attracted spherical sponge iron (99.8%_(wt) pure, ⁻50 to⁺100 mesh). Ingots 14-04-05, 14-04-03, 14-02-06, all exhibited a fairlyrandom patterning (“sprinkling”) of attraction, while ingot 14-03-02appears to have definite “lines” of attraction.

Magnetic Field Testing: Gauss Measurements

In a natural material, the attraction of a magnet or ferromagnet isaccompanied by the appearance of a magnetic field (caused by thealignment of magnetic moments in the magnetic or ferromagnetic materialcreating a measurable field strength, magnetic density or magneticflux). Since each of these tailored materials exhibited an attraction toa Nd/Fe/B magnet (and many attracted ferromagnetic iron), Gauss readingswere taken at designated intervals across the ingot surface to observeany potential magnetic fields (using an F.W. Bell 4048 Gauss Meter). Thedetailed magnetic grids obtained from such testing may be found inAppendix 3. The results are summarized in Table 4 below.

TABLE 4 Gauss Meter Readings Showing No Significant Measurable MagneticFields on Tailored Ingots Maximum Tailored Material Significant AbsoluteExpt'l Run and Experimental Magnetic Gauss Number “Method”/ProtocolField^(†) Reading^(‡,††) 14-04-05 Cu “HD” None 0.0 ± 0.2 14-02-06 Cu“HA” None 0.0 ± 0.2 14-03-02 Cu “AB” None 0.0 ± 0.2 14-01-21 Ni/Re “HD”None 0.0 ± 0.5 14-04-03 Cu/Re/Au/Ag “HD” None 0.0 ± 0.2 ^(†)The averagemagnetic field observed at the earth's surface is between 0.1-0.5 gauss.^(‡)The maximum absolute gauss reading for natural, high purity(99.9%_(wt)) copper was 0.0 ± 0.2. ^(††)The maximum absolute gaussreading for natural, high purity (99.99%_(wt)) nickel was 0.0 ± 0.6.Note, no significant detectable magnetic field was observed on any ofthese tailored ingots despite their ability to attract and hold a magnetat 90° (i.e., vertical orientation). The measured gauss strengths arecomparable to the background levels measured at the earth's surface. Theaverage magnetic field observed at the earth's surface is between0.1-0.5 gauss. Commercially available magnets exhibit gauss strengthsmeasured in the 1000's: Nd/Fe/B magnets 10,500-14,000 gauss, SmCo8,000-12,000 gauss, AlNiCo 6,000-13,500 gauss and Ferrite 2,000-4,000gauss. In addition, the areas exhibiting the greatest apparent magneticforce (0.5 gauss) were tested for attraction to iron filings. No ironfilings held on these particular locations.

The conclusions that can be drawn from this series of documentedattractions:

-   -   Tailored materials exhibit unique attraction to magnetic,        ferromagnetic, and non-magnetic materials that are not observed        in natural materials.    -   Unlike natural materials, tailored materials exhibit no        correlation between observable magnetic field strength (as        measured by a gauss meter) and material attraction (magnetic,        ferromagnetic, or non-magnetic).    -   The unique attraction properties of tailored materials are        attributable to a change in the electromagnetic behavior,        indicative of a change in the composition of matter.    -   These surface attractions are not attributable to surface        irregularities or induced magnetic fields as the tailored        materials:        -   1. Have exhibited unique attraction in the “raw” and            polished state, in multiple positions, and on multiple            surfaces (both internal and external).        -   2. Have attracted fine particles (sulfur and spherical iron            sponge) and large particles (⅛″ diameter magnetic, iron            chips).        -   3. Have exhibited multiple areas of attraction and those            areas attracting sulfur are not necessarily the same areas            that attract ferromagnetic or magnetic materials. Similarly,            areas that attract magnets are not necessarily the areas            that attract ferromagnets or non-magnets.            Exhibit negligible magnetic field strengths as measured by            an F.W. Bell 4048 gauss meter.

-   ¹Zee, A. Quantum Field Theory in a Nutshell. Princeton: Princeton U    P, 2003

-   ²Wen, Xiao-Gang. Quantum Field Theory of Many-Body Systems. New    York: Oxford U P, 2004

-   ³Stormer, Horst, L., Daniel C. Tsui, Arthur C. Gossard. “The    Fractional Quantum Hall Effect.” Reviews of Modern Physics 71.2    (1999): S298-S305

-   ⁴Thurston, William, P. Three-Dimensional Geometry and Topology.    Vol. 1. Princeton: Princeton U P, 1997

-   ⁵Thurston, William, P. The Geometry and Topology of Three-Manifolds.    March 2002. Princeton U P    <http://www.msri.org/publications/books/gt3m>

-   ⁶Nakahara, Mikio. Geometry Topology and Physics. Second Edition.    London: Institute of Physics Publishing, 2003

-   ⁷Nash, Charles. Differential Topology and Quantum Field Theory.    London: Academic P, 1991

-   ⁸Maskit, Bernard. “Moduli of Marked Reimann Surfaces.” Bulletin of    the American Mathematical Society 80.4 (1974): 773-777

-   ⁹Kra, Irwin. “Horocyclic Coordinates for Riemann Surfaces and Moduli    Spaces. 1: Teichmuller and Riemann Spaces of Kleinian Groups.”    Journal of the American Mathematical Society 3.3 (1990): 499-578

-   ¹⁰Keen, Linda, Bernard Maskit, and Caroline Series. Geometric    Finiteness and Uniqueness for Kleinian Groups with Circle Packing    Limit Sets. December 1991. <www.arxiv.org/abs/math/9201299>

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While this invention has been particularly shown and described withreferences to preferred embodiments thereof, it will be understood bythose skilled in the art that various changes in form and details may bemade therein without departing from the scope of the inventionencompassed by the appended claims.

1. A method of modifying the electronic structure of a materialcomprising the steps of: (1.) Melting the material; (2.) Adding a carbonsource to the material; and (3.) Varying the temperature of the materialbetween two temperatures over one or more cycles, wherein the materialremains at a temperature above the melting point during the entire step;and (4) Cooling the material to room temperature; the improvementcomprising exposing at least one gas or gaseous addition to a radiationsource and adding said gas or gaseous addition during one or more of theabove steps; and/or exposing the material to a radiation source induring one or more of the above steps, wherein said radiation source isselected from the group consisting of short arc lamps, high intensitydischarge lamps, pencil lamps, lasers, light emitting diodes, aradiation source emitting wavelengths consisting of infraredwavelengths, a radiation source emitting wavelengths consisting ofultraviolet wavelengths, a radiation source emitting wavelengthsconsisting of long wave ultraviolet wavelengths and/or halogen lamps. 2.The method of claim 1 further comprising one or more of the steps, inone or more iterations or cycles: (5.) Adding a flow of a gas throughthe material; (6.) Varying the temperature of the material between twotemperatures over one or more cycles, wherein the material remains at atemperature above the melting point during the entire step; (7.) Addinga carbon source to the material; and/or (8.) Holding the material withoptional gas addition.
 3. The method of claim 2 further comprising oneor more of the steps, in one or more iterations or cycles: (9.) Loweringthe temperature of a molten material, wherein the material becomessupersaturated with carbon; (10.) Varying the temperature of thematerial between two temperatures over one or more cycles, whereinsupersaturation with carbon is maintained and the material remains at atemperature above the melting point during the entire step, optionallyin the presence of gas addition during the entire step or any portion ofthe step; (11.) Holding the material at a selected temperature,optionally in the presence of gas addition; and/or (12.) Cooling thematerial, such that the material continues to be supersaturated withcarbon and the material remains at a temperature above the meltingpoint, optionally in the presence of gas addition.
 4. The method ofclaim 3 wherein steps 9, 10 and/or 11 are repeated at least one time. 5.The method of claim 3 wherein steps 9, 10 and/or 11 are repeated atleast four times.
 6. The method of claim 1 wherein said gas or gaseousaddition comprises a combination of at least two of the following gases:hydrogen, helium, nitrogen, neon, argon, and krypton.
 7. The method ofclaim 1 wherein the radiation source is a pencil lamp.
 8. The method ofclaim 1 wherein the radiation source is a high intensity discharge lamp.9. The method of claim 1 wherein the radiation source is a short arclamp.
 10. The method of claim 1 wherein multiple radiation sources areused in combination.
 11. The method of claim 1 wherein the improvementcomprises, during step (3), adding a first gas to the material whileincreasing the temperature of the material and adding a second anddifferent gas to the material while decreasing the temperature of thematerial.
 12. The method of claim 11 wherein the first and second gasesare gas mixtures.
 13. The method of claim 12 wherein the first and/orsecond gas mixtures are exposed to radiation.
 14. The method of claim 1wherein the radiation source emits visible light.
 15. The method ofclaim 14 wherein the material is exposed to said radiation source in apulsed sequence.
 16. The method of claim 14 wherein the material isexposed to said radiation source in combination with a filter.
 17. Themethod of claim 1 wherein the radiation source emits a wavelength in therange of 180 nm to 1100 nm.
 18. The method of claim 17 wherein thewavelength is between 400 nm and 700 nm.
 19. The method of claim 1wherein the gas is in a translucent or transparent conduit while exposedto said radiation source in a closed system.
 20. The method of claim 1fun her comprising the step of filtering radiation emitted from at leastone form of the radiation source and exposing the material or at leastone gas to the filtered radiation in a further step or during one ormore of the above steps.
 21. A method of modifying the electronicstructure of a material comprising exposing a material to a radiationsource, wherein the material has been produced by a process comprisingthe steps of: (1.) Melting the material; (2.) Adding a carbon source tothe material; and (3.) Varying the temperature of the material betweentwo temperatures over one or more cycles, wherein the material remainsat a temperature above the melting point during the entire step; and (4)Cooling the material to room temperature wherein said radiation sourceis selected from the group consisting of short arc lamps, high intensitydischarge lamps, pencil lamps, lasers, light emitting diodes, aradiation source emitting wavelengths consisting of infraredwavelengths, a radiation source emitting wavelengths consisting ofultraviolet wavelengths, a radiation source emitting wavelengthsconsisting of long wave ultraviolet wavelengths and/or halogen lamps.